A total of six three-dimensional chiral coordination compounds L- and D-[LnZn(IN)(3)(C2H4O2)](n) (Ln = Eu, Sm, and Gd; HIN = isonicotinic acid) have been successfully synthesized under hydrothermal conditions without any chiral auxiliary and characterized by IR, TG, elemental analyses, and solid-state circular dichroism spectra. The structures of 1-6 were determined by single-crystal X-ray structural analysis, which shows that L-[LnZn(IN)(3)(C2H4O2)](n) (Ln = Eu (1), Sm (2), and Gd (3)) crystallize in space group P6(5)22 and are levogyrate. The chiral frameworks of L-[LnZn(IN)(3)(C2H4O2)](n) are constructed from L-helical Ln-O-Zn cluster chains, while adjacent L-type helical -[Ln-O-Zn](n)- chains are connected through IN- ligands. D-[LnZn(IN)(3)(C2H4O2)](n) (Ln = Eu (4), Sm (5), and Gd (6)) crystallize in space group P6(1)22, and their chiral frameworks consist of n-helical Ln-O-Zn cluster chains. The observed second-harmonic generation efficiencies of [EuZn(IN)(3)(C2H4O2)](n), [SmZn(IN)(3)(C2H4O2)](n), and [GdZn(IN)(3)-(C2H4O2)](n) are 0.4, 0.3, and 0.3 times that of urea, respectively. We also studied luminescence spectra and luminescence lifetimes of 1 and 2. The luminescence lifetimes of 1 and 2 are 1.18 ms, and 29.6 mu s, respectively.