alpha-Amino nitriles are synthesized by a one-pot three-component condensation reaction of amines, aldehydes and trimethylsilylcyanide in the presence of a catalytic amount of cellulose sulfuric acid as a bio-supported catalyst, in excellent yields with short reaction times at ambient temperature. The reaction work-up is simple and the catalyst can be easily separated from the product and reused in subsequent reactions. (C) 2007 Elsevier B.V. All rights reserved.