It is prepared by the reaction of lithium cyanide and trimethylsilyl chloride:[1][2] The molecule exhibits the structure of a nitrile-like compound.

The compound exists in a rapid equilibrium with a small amount of the isomeric isocyanide (CH3)3SiNC.

[4] Trimethylsilyl cyanide hydrolyzes to give hydrogen cyanide and trimethylsilanol: In its principal application, it adds across carbon-oxygen double bonds, for example in an aldehyde, to form a new carbon-carbon bond:[2] The product is an O-silylated cyanohydrin.

This transformation is best done in dichloromethane solution using dimethylcarbamoyl chloride as the activating electrophile.

It is possible to use benzoyl chloride but the yields and regioselectivity of the addition of the cyano group are lower.