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An efficient preparation of the girgensohnine and its close analogs with α-aminonitrile structure, and their spectral characterization were reported for the first time. The piperidine α-aminonitriles were obtained through 5 mol% InCl3-catalyzed one-pot Strecker reaction, and tested for antioxidant activity and AChE inhibitory properties. It was found that girgensohnine possesses a moderate AChE inhibitory property while its spiroanalog shows good antioxidant capacity.