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

    <schemaVersion>X0306</schemaVersion>

    <documentType>4</documentType>

    <periodOfReport>2016-05-18</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 200</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></nonDerivativeTable>

    <derivativeTable>
        <derivativeTransaction>
            <securityTitle>
                <value>Restricted Stock Units</value>
            </securityTitle>
            <conversionOrExercisePrice>
                <footnoteId id="F1"/>
            </conversionOrExercisePrice>
            <transactionDate>
                <value>2016-05-18</value>
            </transactionDate>
            <transactionCoding>
                <transactionFormType>4</transactionFormType>
                <transactionCode>A</transactionCode>
                <equitySwapInvolved>0</equitySwapInvolved>
            </transactionCoding>
            <transactionAmounts>
                <transactionShares>
                    <value>21000</value>
                </transactionShares>
                <transactionPricePerShare>
                    <footnoteId id="F1"/>
                </transactionPricePerShare>
                <transactionAcquiredDisposedCode>
                    <value>A</value>
                </transactionAcquiredDisposedCode>
            </transactionAmounts>
            <exerciseDate>
                <value>2017-04-01</value>
            </exerciseDate>
            <expirationDate>
                <footnoteId id="F2"/>
            </expirationDate>
            <underlyingSecurity>
                <underlyingSecurityTitle>
                    <value>Common Stock</value>
                </underlyingSecurityTitle>
                <underlyingSecurityShares>
                    <value>21000.0</value>
                </underlyingSecurityShares>
            </underlyingSecurity>
            <postTransactionAmounts>
                <sharesOwnedFollowingTransaction>
                    <value>21000</value>
                </sharesOwnedFollowingTransaction>
            </postTransactionAmounts>
            <ownershipNature>
                <directOrIndirectOwnership>
                    <value>D</value>
                </directOrIndirectOwnership>
            </ownershipNature>
        </derivativeTransaction>
        <derivativeTransaction>
            <securityTitle>
                <value>Performance Based Restricted Stock Units</value>
            </securityTitle>
            <conversionOrExercisePrice>
                <footnoteId id="F3"/>
            </conversionOrExercisePrice>
            <transactionDate>
                <value>2016-05-18</value>
            </transactionDate>
            <transactionCoding>
                <transactionFormType>4</transactionFormType>
                <transactionCode>A</transactionCode>
                <equitySwapInvolved>0</equitySwapInvolved>
            </transactionCoding>
            <transactionAmounts>
                <transactionShares>
                    <value>35000</value>
                </transactionShares>
                <transactionPricePerShare>
                    <footnoteId id="F3"/>
                </transactionPricePerShare>
                <transactionAcquiredDisposedCode>
                    <value>A</value>
                </transactionAcquiredDisposedCode>
            </transactionAmounts>
            <exerciseDate>
                <value>2019-04-01</value>
            </exerciseDate>
            <expirationDate>
                <value>2019-04-01</value>
            </expirationDate>
            <underlyingSecurity>
                <underlyingSecurityTitle>
                    <value>Common Stock</value>
                </underlyingSecurityTitle>
                <underlyingSecurityShares>
                    <value>52500.0</value>
                    <footnoteId id="F3"/>
                </underlyingSecurityShares>
            </underlyingSecurity>
            <postTransactionAmounts>
                <sharesOwnedFollowingTransaction>
                    <value>35000</value>
                </sharesOwnedFollowingTransaction>
            </postTransactionAmounts>
            <ownershipNature>
                <directOrIndirectOwnership>
                    <value>D</value>
                </directOrIndirectOwnership>
            </ownershipNature>
        </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">Each Performance Based Restricted Stock Unit represents a contingent right to receive up to 1.5 shares of common stock. The units vest over approximately three years and become payable on April 1, 2019; 25% weighted based on a comparison of the company's relative total shareholder return over the vesting period to a weighted total shareholder return during such period of companies in the Russell 3000 Index; 25% weighted based on a comparison of the company's relative total shareholder return over the vesting period to a weighted total shareholder return during such period of certain companies in the Market Vectors Global Coal Index with principal places of business in the US, Australia or Canada; and 50% weighted based on a three-year free cash flow goal for Westmoreland's consoldated global enterprise.</footnote>
    </footnotes>

    <remarks></remarks>

    <ownerSignature>
        <signatureName>Jennifer S. Grafton by Power of Attorney</signatureName>
        <signatureDate>2016-05-20</signatureDate>
    </ownerSignature>
</ownershipDocument>
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X0306
4
2016-05-18
0
0000106455
WESTMORELAND COAL Co
WLB
0001615056
Schadan John Alexander
9540 SOUTH MAROON CIRCLE, SUITE 200
ENGLEWOOD
CO
80112
0
1
0
0
Chief Operating Officer
Restricted Stock Units
2016-05-18
4
A
0
21000
A
2017-04-01
Common Stock
21000.0
21000
D
Performance Based Restricted Stock Units
2016-05-18
4
A
0
35000
A
2019-04-01
2019-04-01
Common Stock
52500.0
35000
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.
Each Performance Based Restricted Stock Unit represents a contingent right to receive up to 1.5 shares of common stock. The units vest over approximately three years and become payable on April 1, 2019; 25% weighted based on a comparison of the company's relative total shareholder return over the vesting period to a weighted total shareholder return during such period of companies in the Russell 3000 Index; 25% weighted based on a comparison of the company's relative total shareholder return over the vesting period to a weighted total shareholder return during such period of certain companies in the Market Vectors Global Coal Index with principal places of business in the US, Australia or Canada; and 50% weighted based on a three-year free cash flow goal for Westmoreland's consoldated global enterprise.
Jennifer S. Grafton by Power of Attorney
2016-05-20