A new catalyst type for a new reaction. The unprecedented cyanosilylation of nitroalkenes can be efficiently catalyzed by a bifunctional quinine derivative bearing tetra-alkylammonium cyanide and thiourea moieties. The activation of the nitroalkene by H-bonding to the thiourea together with the presence of an "active" cyanide provide a new mode of activation leading to products in high yields and good selectivities.