The high surface area three-dimensional porous catalyst has been prepared and characterized by TEM. BET S.A, low angle XRD, Si-29 MAS NMR, NH3 TPD techniques. A simple, efficient and rapid method for the green synthesis of alpha-aminonitriles has been demonstrated over a new mesoporous gallosilicate catalyst Ga-TUD-1. The solventless technique has been applied for the synthesis of a range of compounds with variable functionality with excellent yield and selectivity. The catalyst has been recycled four times with reproducible yield. (C) 2010 Elsevier B.V. All rights reserved.