Chiral organic-inorganic metal halide (OIMH) materials are gaining increasing attention as candidates for asymmetric materials due to their unique photoelectric, chiral optic, and spintronic properties. The introduction of chirality into OIMHs is usually achieved by the use of chiral organic cations, while previous studies often focus on primary ammonium cations derived from commercially available chiral amines, limiting the tunability of the OIMH materials. Herein, we report the use of Zincke reactions to synthesize chiral N-substituted pyridinium salts, namely, (R)/(S)-methylbenzylpyridinium (