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The reactivity of sulfido ligands with different coordination configurations are systematically introduced leading to "unit construction", as a convenient method for designed synthesis of some heterometallic copper(silver)-sulfur cluster compounds. Heterometallic copper(silver)-sulfur cluster crystals with acentric space groups as potential precursors of crystal materials with non-linear physical properties are discussed. Discussions of synthetic methods and crystal structures for larger M-Cu-S cluster derivatives containing a square-type unit {M4Cu4S12} (M = Mo, W) are also provided. Additionally, polymeric M-Ag-S cluster complexes and the coexistence of polymeric cluster anions and hydrogen-bond supramolecular structure cations are rudimentarily explored.In recent years, the synthetic and structural chemistry of heterometallic copper (silver)-sulfur cluster compounds has developed rapidly (7). There are at least three factors stimulating this rapid development; i) the biological Mo-Cu antagonism (2-5) and the desire to produce analogues of active sites of metal enzymes (4); ii) the rich structural variety of complexes of this kind (1-4); iii) the nonlinear optical properties of transition metal sulfido cluster compounds (5-8).