Two new semiconducting zinc coordination polymers, Zn8S(SPh)(14)(bpy) (1) and Zn-2(SPh)(4)(bpy) (2), have been synthesized by a dual-ligand approach. Single-crystal structural analyses indicate that compound 1 has a helical-chain structure with PI clusters bridging with bipyridyl (bpy) ligands and compound 2 possesses a layered structure with zinc sulfide chains cross-linked with bpy ligands. The diffuse-reflectance spectra reveal that the band gaps of the two compounds are 2.41 eV for 1 and 2.56 eV for 2.