The efficient and novel approach for synthesizing cyanomethylated thiohydantoin from readily obtainable acetonitrile and 1,3-dibenzyl-2-thiohydantoin through iron(II)-catalyzed cross dehydrogenative coupling (CDC) protocol is documented here. The strategy displays extensive substrate scope, and provides an effectual construction of cyanomethylated thiohydantoins in moderate to good yield. Prominently, this new methodology represents hitherto unobserved reactivity pattern for the thiohydantoin.

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