A series of PbII coordination polymers [Pb(ndc)(dpp)] (1), [Pb(ndc)(ptcp)]⋅0.5 H2O (2), [Pb(ndc)(dppz)] (3), [Pb(ndc)(tcpn)2] (4), [Pb2(ndc)2(tcpp)] (5), [Pb(Hndc)2]⋅H2O (6), [Pb(ndc)(dma)] (7), [Pb(bdc)(dma)] (8), [Pb(trans-chdc)(H2O)] (9), and [Pb2(cis-chdc)2]⋅NH(CH3)2 (10), where ndc=1,4-naphthalenedicarboxylate, dpp=4,7-diphenyl-1,10-phenanthroline, ptcp=2-phenyl-1H-1,3,7,8-tetraazacyclopenta[l]phenanthrene, dppz=dipyrido[3,2-a:2′,3′-c]phenazine, tcpn=2-(1H-1,3,7,8-tetraazacyclopenta[l]phenanthren-2-yl)naphthol, tcpp=4-(1H-1,3,7,8-tetraazacyclopenta[l]phenanthren-2-yl)phenol, dma=N,N-dimethylacetamide, bdc=1,4-benzenedicarboxylate, and chdc=1,4-cyclohexanedicarboxylate, have been synthesized from a hydrothermal or solvothermal reaction system by varying the ligands or the solvents. Compounds 1–5 crystallize with an N-donor chelating ligand and an aromatic dicarboxylate linker. Compounds 1–4 are 1D polymers with different π–π stacking interactions, whereas compound 5 consists of 2D layers. The structures of compounds 7, 8, and 10 are 3D frameworks formed by connection of the PbII centers by organic acid ligands. Compound 7 is chiral although the ndc ligand is achiral, while the framework of 8 is a typical 3D (3,4)-connected net. Compound 10 is the first example of PbII wheel cluster [Pb8O8] units bridged by carboxylate groups. Compound 6 contains 1D chains which are further extended to a 3D structure by π–π interactions. Compound 9 consists of a 2D network constructed by PbII centers and trans-chdc ligands. The structural differences between 7 and 8 and between 9 and 10 indicate the importance of solvents for framework formation of the coordination polymers. By varying the solvent the cis and trans conformations of H2chdc in 9 and 10 were separated completely. The photoluminescence and nonlinear optical properties of the coordination polymers have also been investigated.