Chiral hybrid metal halides have grabbed extensive attention in linear and nonlinear chiroptics. Herein, 0D chiral zinc halides, (R-/S-2-MP)ZnCl4, have been fabricated, which demonstrate high efficiency second-order nonlinear optical responses. Incorporating Sb3+ into the chiral zinc halide matrix triggers the circularly polarized luminescence effectively with a balance between quantum yield and luminescence dissymmetry factor.