In the presence of a catalytic amount of chiral oxazaborolidinium ion (COBI), aldimine reacted with trimethylsilyl cyanide (TMSCN) to a afford α-aminonitriles in excellent yields and enantioselectivities. The three-component asymmetric process studied here significantly improves upon the original Strecker reaction, and has advantages over previous reactions using unstable imines. High levels of enantioselectivities in the synthesis of α-aminonitrile derivatives with wide substrate generality were obtained via these reactions. The reaction proceeded in good yields (up to 98%) with excellent enantioselectivities (up to 97% ee).