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Piezoelectricity, one of the most desirable properties of non-centrosymmetric crystalline materials, has long been blooming in academic research, industrial manufacturing, and daily applications owing to its unique electromechanical transformation capability. Compared with inorganic piezoelectric ceramics dominating the market, molecule-based piezoelectric materials exhibit advantages of light weight, mechanical flexibility, and environment friendliness and have attracted widespread interest recently. However, investigations on molecular materials with large piezoelectric coefficients are mainly focused on organic–inorganic hybrids, while pure organic homochiral piezoelectrics holding large piezoelectric coefficients remain scarce. Herein, by precise molecular modification on (S)-2-methylpiperazin-1-ium perchlorate ([(S)-MPP][ClO4]) with polar cyanomethyl groups, a homochiral pure organic compound (3S)-3-methyl-1,4-di(cyanomethyl)piperazin-1-ium perchlorate [DCM-(S)-MPP][ClO4] with large d22 of 18 pC/N was achieved, along with changes in the space group from nonpolar to polar, giving rise to second harmonic generation and phase transition behaviors. The modification strategy proposed here will benefit piezoelectricity enhancement in more chiral compounds, promoting their application potential in biological medicine, flexible devices, and green chemistry. [ABSTRACT FROM AUTHOR]