The role of anions in the formation of diversified coordination polymers (CPs) of a flexible bidentate ligand (L), containing an aliphatic-aromatic spacer (p-xylyl) between amidopyridine moieties, has been explored. The reaction of L with Cd(II) or Cu(II) salts of NO3–, ClO4–, SO42–, and SiF62– resulted in the single crystals of eight CPs. The X-ray diffraction analyses of the single crystals reveal that the CPs contain 1D-zigzag (SiF62–), open (4,4)-network (NO3– and SCN–), and the interpenetrated 2D-networks with (4,4)- and (6,3)-topologies and pseudodiamondoid network (SO42– and ClO4–). These results clearly indicate that the presence of tetrahedral anions favored the interpenetration of the 2D- and 3D-networks. The resultant cationic CPs are explored for their dye adsorption ability based on the charge transfer interaction between the framework and ionic dye. Among all CPs, complex 8 containing a 3D-interpenetrated diamondoid network was found to show remarkable ability for the uptake of anionic dyes ...