The action of concentrated sulfuric acid upon unsaturated aliphatic isothiocyanates has been investigated only slightly. Allyl isothiocyanate is reported to yield allylamine sulfate. However, we have found that the presence of a double bond carrying a tertiary carbon atom, as in methallyl isothiocyanate (I) or in methyl methallyl isothiocyanate (XII) leads to the formation of more complex substances, namely, mercaptothiazolines.