A convenient and efficient one-pot method for the synthesis of a variety of α-amino nitriles from aldehydes, amines and trimethylsilyl cyanide (TMSCN) in the presence of a catalytic amount of Bi(NO3)3 at room temperature in acetonitrile (MeCN) is described. The significant features of this method are simple work-up procedure, inexpensive and non-toxic catalyst, shorter reaction times and excellent product yields. The catalyst Bi(NO3)3 can be reused. The reusability of the catalyst has been studied for the synthesis of various amino nitriles.