In this work, a green and cost-effective method based on halloysite as natural catalyst for the synthesis of α-amino nitriles via Strecker three-component reaction is introduced. The chemical and physical structure of natural halloysite has characterized thoroughly, and then the effect of different parameters such as the amount of catalyst, solvent, and temperature was optimized in the synthesis of 2-phenyl-2-(phenylamino)acetonitrile as the model reaction. Then, various substituted benzaldehydes and anilines were converted to the desired α‐amino nitriles under the optimized conditions. Electronic properties of substituents on aldehydes and aromatic amines have been affected the reaction efficiency. For all substrates, good to excellent yields of the corresponding α-amino nitriles were obtained under solvent-free conditions at room temperature. The catalyst has been recovered and reused five times in successive Strecker reaction.

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