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One-pot synthesis of cyanamides from isoselenocyanates through deselenisation promoted by ionic liquid-supported hypervalent iodine(III) reagent 1-(4-diacetoxyiodobenzyl)-3-methylimidazolium tetrafluoroborate ([dibmim]+[BF4]−) was developed. This approach provided a simple, mild and environmentally benign way to construct cyanamides in good yields. Moreover, powder Se and [dibmim]+[BF4]− could be easily recycled. It was the first example of [dibmim]+[BF4]− to be used as a deselenising agent.

This method gives also access to α‐keto amides.

The one‐pot synthesis of various cyanamides involves a deselenisation mediated by an ionic liquid‐supported hypervalent iodine(III) reagent.