<?xml version="1.0"?>
<ownershipDocument>

    <schemaVersion>X0306</schemaVersion>

    <documentType>4</documentType>

    <periodOfReport>2017-04-13</periodOfReport>

    <notSubjectToSection16>0</notSubjectToSection16>

    <issuer>
        <issuerCik>0000106455</issuerCik>
        <issuerName>WESTMORELAND COAL Co</issuerName>
        <issuerTradingSymbol>WLB</issuerTradingSymbol>
    </issuer>

    <reportingOwner>
        <reportingOwnerId>
            <rptOwnerCik>0001615056</rptOwnerCik>
            <rptOwnerName>Schadan John Alexander</rptOwnerName>
        </reportingOwnerId>
        <reportingOwnerAddress>
            <rptOwnerStreet1>9540 SOUTH MAROON CIRCLE, SUITE 300</rptOwnerStreet1>
            <rptOwnerStreet2></rptOwnerStreet2>
            <rptOwnerCity>ENGLEWOOD</rptOwnerCity>
            <rptOwnerState>CO</rptOwnerState>
            <rptOwnerZipCode>80112</rptOwnerZipCode>
            <rptOwnerStateDescription></rptOwnerStateDescription>
        </reportingOwnerAddress>
        <reportingOwnerRelationship>
            <isDirector>0</isDirector>
            <isOfficer>1</isOfficer>
            <isTenPercentOwner>0</isTenPercentOwner>
            <isOther>0</isOther>
            <officerTitle>Chief Operating Officer</officerTitle>
            <otherText></otherText>
        </reportingOwnerRelationship>
    </reportingOwner>

    <nonDerivativeTable>
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            <securityTitle>
                <value>Common Stock</value>
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                </transactionShares>
                <transactionPricePerShare>
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                </transactionPricePerShare>
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                    <value>A</value>
                </transactionAcquiredDisposedCode>
            </transactionAmounts>
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                <sharesOwnedFollowingTransaction>
                    <value>3966</value>
                </sharesOwnedFollowingTransaction>
            </postTransactionAmounts>
            <ownershipNature>
                <directOrIndirectOwnership>
                    <value>D</value>
                </directOrIndirectOwnership>
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            <securityTitle>
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                </transactionShares>
                <transactionPricePerShare>
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                </transactionPricePerShare>
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                </transactionAcquiredDisposedCode>
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                </sharesOwnedFollowingTransaction>
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            <securityTitle>
                <value>Common Stock</value>
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            <transactionDate>
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                </directOrIndirectOwnership>
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        <nonDerivativeTransaction>
            <securityTitle>
                <value>Common Stock</value>
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            <transactionDate>
                <value>2017-04-13</value>
            </transactionDate>
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            <securityTitle>
                <value>Common Stock</value>
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            <transactionDate>
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                <transactionFormType>4</transactionFormType>
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                <equitySwapInvolved>0</equitySwapInvolved>
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                <transactionShares>
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                </transactionPricePerShare>
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                </transactionAcquiredDisposedCode>
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            <securityTitle>
                <value>Common Stock</value>
            </securityTitle>
            <transactionDate>
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                <transactionFormType>4</transactionFormType>
                <transactionCode>F</transactionCode>
                <equitySwapInvolved>0</equitySwapInvolved>
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            <transactionAmounts>
                <transactionShares>
                    <value>3367</value>
                </transactionShares>
                <transactionPricePerShare>
                    <value>0</value>
                </transactionPricePerShare>
                <transactionAcquiredDisposedCode>
                    <value>D</value>
                </transactionAcquiredDisposedCode>
            </transactionAmounts>
            <postTransactionAmounts>
                <sharesOwnedFollowingTransaction>
                    <value>8685</value>
                </sharesOwnedFollowingTransaction>
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            <ownershipNature>
                <directOrIndirectOwnership>
                    <value>D</value>
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            </ownershipNature>
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        <nonDerivativeTransaction>
            <securityTitle>
                <value>Common Stock</value>
            </securityTitle>
            <transactionDate>
                <value>2017-04-13</value>
            </transactionDate>
            <transactionCoding>
                <transactionFormType>4</transactionFormType>
                <transactionCode>M</transactionCode>
                <equitySwapInvolved>0</equitySwapInvolved>
            </transactionCoding>
            <transactionAmounts>
                <transactionShares>
                    <value>4823</value>
                </transactionShares>
                <transactionPricePerShare>
                    <value>0</value>
                </transactionPricePerShare>
                <transactionAcquiredDisposedCode>
                    <value>A</value>
                </transactionAcquiredDisposedCode>
            </transactionAmounts>
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                <sharesOwnedFollowingTransaction>
                    <value>13508</value>
                </sharesOwnedFollowingTransaction>
            </postTransactionAmounts>
            <ownershipNature>
                <directOrIndirectOwnership>
                    <value>D</value>
                </directOrIndirectOwnership>
            </ownershipNature>
        </nonDerivativeTransaction>
        <nonDerivativeTransaction>
            <securityTitle>
                <value>Common Stock</value>
            </securityTitle>
            <transactionDate>
                <value>2017-04-13</value>
            </transactionDate>
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                <transactionFormType>4</transactionFormType>
                <transactionCode>F</transactionCode>
                <equitySwapInvolved>0</equitySwapInvolved>
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            <transactionAmounts>
                <transactionShares>
                    <value>2248</value>
                </transactionShares>
                <transactionPricePerShare>
                    <value>14.61</value>
                </transactionPricePerShare>
                <transactionAcquiredDisposedCode>
                    <value>D</value>
                </transactionAcquiredDisposedCode>
            </transactionAmounts>
            <postTransactionAmounts>
                <sharesOwnedFollowingTransaction>
                    <value>11260</value>
                </sharesOwnedFollowingTransaction>
            </postTransactionAmounts>
            <ownershipNature>
                <directOrIndirectOwnership>
                    <value>D</value>
                </directOrIndirectOwnership>
            </ownershipNature>
        </nonDerivativeTransaction>
    </nonDerivativeTable>

    <derivativeTable>
        <derivativeTransaction>
            <securityTitle>
                <value>Restricted Stock Units</value>
            </securityTitle>
            <conversionOrExercisePrice>
                <footnoteId id="F1"/>
            </conversionOrExercisePrice>
            <transactionDate>
                <value>2017-04-13</value>
            </transactionDate>
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                <transactionFormType>4</transactionFormType>
                <transactionCode>M</transactionCode>
                <equitySwapInvolved>0</equitySwapInvolved>
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            <transactionAmounts>
                <transactionShares>
                    <value>1072</value>
                </transactionShares>
                <transactionPricePerShare>
                    <footnoteId id="F1"/>
                </transactionPricePerShare>
                <transactionAcquiredDisposedCode>
                    <value>D</value>
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            </transactionAmounts>
            <exerciseDate>
                <value>2015-04-01</value>
            </exerciseDate>
            <expirationDate>
                <footnoteId id="F2"/>
            </expirationDate>
            <underlyingSecurity>
                <underlyingSecurityTitle>
                    <value>Common Stock</value>
                </underlyingSecurityTitle>
                <underlyingSecurityShares>
                    <value>1072.0</value>
                </underlyingSecurityShares>
            </underlyingSecurity>
            <postTransactionAmounts>
                <sharesOwnedFollowingTransaction>
                    <value>0</value>
                </sharesOwnedFollowingTransaction>
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            <ownershipNature>
                <directOrIndirectOwnership>
                    <value>D</value>
                </directOrIndirectOwnership>
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            <transactionDate>
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                <transactionFormType>4</transactionFormType>
                <transactionCode>M</transactionCode>
                <equitySwapInvolved>0</equitySwapInvolved>
            </transactionCoding>
            <transactionAmounts>
                <transactionShares>
                    <value>2819</value>
                </transactionShares>
                <transactionPricePerShare>
                    <footnoteId id="F1"/>
                </transactionPricePerShare>
                <transactionAcquiredDisposedCode>
                    <value>D</value>
                </transactionAcquiredDisposedCode>
            </transactionAmounts>
            <exerciseDate>
                <value>2016-04-01</value>
            </exerciseDate>
            <expirationDate>
                <footnoteId id="F2"/>
            </expirationDate>
            <underlyingSecurity>
                <underlyingSecurityTitle>
                    <value>Common Stock</value>
                </underlyingSecurityTitle>
                <underlyingSecurityShares>
                    <value>2819.0</value>
                </underlyingSecurityShares>
            </underlyingSecurity>
            <postTransactionAmounts>
                <sharesOwnedFollowingTransaction>
                    <value>2819</value>
                </sharesOwnedFollowingTransaction>
            </postTransactionAmounts>
            <ownershipNature>
                <directOrIndirectOwnership>
                    <value>D</value>
                </directOrIndirectOwnership>
            </ownershipNature>
        </derivativeTransaction>
        <derivativeTransaction>
            <securityTitle>
                <value>Restricted Stock Units</value>
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            <conversionOrExercisePrice>
                <footnoteId id="F1"/>
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            <transactionDate>
                <value>2017-04-13</value>
            </transactionDate>
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                <transactionFormType>4</transactionFormType>
                <transactionCode>M</transactionCode>
                <equitySwapInvolved>0</equitySwapInvolved>
            </transactionCoding>
            <transactionAmounts>
                <transactionShares>
                    <value>7000</value>
                </transactionShares>
                <transactionPricePerShare>
                    <footnoteId id="F1"/>
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                <transactionAcquiredDisposedCode>
                    <value>D</value>
                </transactionAcquiredDisposedCode>
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            <exerciseDate>
                <value>2017-04-01</value>
            </exerciseDate>
            <expirationDate>
                <footnoteId id="F2"/>
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            <underlyingSecurity>
                <underlyingSecurityTitle>
                    <value>Common Stock</value>
                </underlyingSecurityTitle>
                <underlyingSecurityShares>
                    <value>7000.0</value>
                </underlyingSecurityShares>
            </underlyingSecurity>
            <postTransactionAmounts>
                <sharesOwnedFollowingTransaction>
                    <value>14000</value>
                </sharesOwnedFollowingTransaction>
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            <ownershipNature>
                <directOrIndirectOwnership>
                    <value>D</value>
                </directOrIndirectOwnership>
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        </derivativeTransaction>
        <derivativeTransaction>
            <securityTitle>
                <value>Restricted Stock Units</value>
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            <conversionOrExercisePrice>
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            <transactionDate>
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                <transactionCode>M</transactionCode>
                <equitySwapInvolved>0</equitySwapInvolved>
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                    <value>4823</value>
                    <footnoteId id="F3"/>
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                    <footnoteId id="F1"/>
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                <transactionAcquiredDisposedCode>
                    <value>D</value>
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                <value>2017-04-01</value>
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            <expirationDate>
                <value>2017-04-13</value>
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                <underlyingSecurityTitle>
                    <value>Common Stock</value>
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                <underlyingSecurityShares>
                    <value>4823.0</value>
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                <sharesOwnedFollowingTransaction>
                    <value>0</value>
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            <ownershipNature>
                <directOrIndirectOwnership>
                    <value>D</value>
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        </derivativeTransaction>
    </derivativeTable>

    <footnotes>
        <footnote id="F1">Each Restricted Stock Unit represents a contingent right to receive one share of common stock payable in common stock, cash or a combination thereof at the discretion of the Compensation and Benefits Committee.</footnote>
        <footnote id="F2">The Restricted Stock Units vest in three equal annual installments beginning on April 1st following the grant date.</footnote>
        <footnote id="F3">Performance-based Restricted Stock Units granted pursuant to the Westmoreland Coal Company 2014 Equity Incentive Plan for Employees and Non-Employee Directors on June 2, 2014. This award was based on a three year cumulative free cash flow metric and was earned at the maximum of 150% of target grant.</footnote>
    </footnotes>

    <remarks></remarks>

    <ownerSignature>
        <signatureName>/s/ Jennifer S. Grafton by Power of Attorney</signatureName>
        <signatureDate>2017-04-18</signatureDate>
    </ownerSignature>
</ownershipDocument>
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X0306
4
2017-04-13
0
0000106455
WESTMORELAND COAL Co
WLB
0001615056
Schadan John Alexander
9540 SOUTH MAROON CIRCLE, SUITE 300
ENGLEWOOD
CO
80112
0
1
0
0
Chief Operating Officer
Common Stock
2017-04-13
4
M
0
1072
0
A
3966
D
Common Stock
2017-04-13
4
F
0
447
14.61
D
3519
D
Common Stock
2017-04-13
4
M
0
2819
0
A
6338
D
Common Stock
2017-04-13
4
F
0
1286
0
D
5052
D
Common Stock
2017-04-13
4
M
0
7000
0
A
12052
D
Common Stock
2017-04-13
4
F
0
3367
0
D
8685
D
Common Stock
2017-04-13
4
M
0
4823
0
A
13508
D
Common Stock
2017-04-13
4
F
0
2248
14.61
D
11260
D
Restricted Stock Units
2017-04-13
4
M
0
1072
D
2015-04-01
Common Stock
1072.0
0
D
Restricted Stock Unit
2017-04-13
4
M
0
2819
D
2016-04-01
Common Stock
2819.0
2819
D
Restricted Stock Units
2017-04-13
4
M
0
7000
D
2017-04-01
Common Stock
7000.0
14000
D
Restricted Stock Units
2017-04-13
4
M
0
4823
D
2017-04-01
2017-04-13
Common Stock
4823.0
0
D
Each Restricted Stock Unit represents a contingent right to receive one share of common stock payable in common stock, cash or a combination thereof at the discretion of the Compensation and Benefits Committee.
The Restricted Stock Units vest in three equal annual installments beginning on April 1st following the grant date.
Performance-based Restricted Stock Units granted pursuant to the Westmoreland Coal Company 2014 Equity Incentive Plan for Employees and Non-Employee Directors on June 2, 2014. This award was based on a three year cumulative free cash flow metric and was earned at the maximum of 150% of target grant.
/s/ Jennifer S. Grafton by Power of Attorney
2017-04-18