Optically active crystalline polymers have shear piezoelectricity owing to their asymmetric crystal structure. In this study, to explore a novel shear piezoelectric polymer, we have focused on an imide ring structure and synthesized optically active polysuccinimides (PSIs), the minimum structure of optically active polyimides. As a result, optically active PSIs were obtained, and we observed that oriented optically active PSI films show shear piezoelectricity. Furthermore, both optical purity and molecular weight are significant factors in piezoelectric performance. This is the first report of the shear piezoelectricity of optically active polyimides, and we identify herein a novel category of a shear piezoelectric polymer.