3-Phenyl-and 3-unsubstituted-2-alkenoyl-1-methylaziridines have been synthesized via Grignard reactions with the corresponding 2-cyanoaziridines. The 3-phenylated-2- alkenoylaziridines have been thermally transformed into ring-fused pyrrolidine compounds. The configurations and conformations of the aziridine and pyrrolidine compounds have been determined by'H and 13C NMR spectroscopy and X-ray crystallography.