We herein report five coordination polymers (CPs) and two supramolecular cages based on [MS4Cux]x-2 (M = W, Mo, x = 1, 2, … 6) units and N-containing ligands, 9,10-di(1H-imidazol-1-yl)anthracene (dia), 1,6-di(1H-imidazol-1-yl)pyrene (dip), and 1,1',1''-(benzene-1,3,5-triyltris(methylene))tris(1,4-diazabicyclo[2.2.2]octan-1-ium) bromide (bmd), and 1,1',1''-((2,4,6-trimethylbenzene-1,3,5-triyl)tris(methylene))tris(1,4-diazabicyclo[2.2.2]octan-1-ium) (mbmd). Compound 1 and 2 both contained penta-nuclear [(WS4)Cu4]2+ cluster unit. The four Cu+ atoms were arranged in a distorted tetrahedron and rectangle around the (WS4)2- core in 1 and 2, respectivley, and affording a 3-connected unit in 1 and a 2-connected unit in 2. Compound 3, 4 and 5 were built with tri-topic organic ligand bmd, 3 and 4 contained penta-nuclear [WS4Cu4]2+ units, and 5 contained hexa-nuclear [MoS4Cu5]3+ unit, but the connectives of the cluster units in 3, 4 and 5 and the final helical chain structures were similar. Compound 6 contained a tetra-nuclear [WS4Cu3I3]2- unit and positively charged mbmd ligand, the mbmd ligand was in a cis-conformation leading to a supramolecular cage which accommodated a I- anion as guest. 7 is isostructural to 6 but contained [WS4Cu3Cl3]2- cluster unit, mbmd ligand and Br- free anion. This work demonstrated that the number and arrangement of Cu+ around (MS4)2- core can be varied with the synthesis conditions, affording heterothiometallic [(MS4)Cux]x-2 cluster units of versatile geometries and connectivities for building CPs.