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With different transition metal (TM) complexes as structure directing agents or building units, three new multinary chalcognidometalates based on T3 supertetrahedral nanocluster of [Mn2Ga4Sn4S20]8− have been solvothermally synthesized and structurally characterized. In compound Mn2Ga4Sn4S20[Mn2(en)5]2·4H2O (1, en = ethylenediamine), the neighboring [Mn2Ga4Sn4S20]8− cores were bridged by two pairs of [Mn2(en)5]4+ complex cations via Mn–S bonds to form one-dimensional (1D) neutral chains. Compound Mn2Ga4Sn4S20[Mn(dien)2]4·2H2O (2, dien = diethylenetriamine) contained discrete [Mn2Ga4Sn4S20]8− cores separated by [Mn(dien)2]2+ cations. In compound Mn2Ga4Sn4S20[Mn(teta)]4 (3, teta = triethylenetetramine), each [Mn2Ga4Sn4S20]8− core was covalently attached by four [Mn(teta)]2+ complexes via terminal Mn–S bonds to form a neutral isolated cluster. The photocatalytic experiments indicate that compound 1 was able to degrade rhodamine B (RhB) and crystal violet (CV) under visible irradiation. Furthermore, the luminescence properties and thermal stabilities of the title compounds, as well as the second-order nonlinear optical property of 3 were also studied. [ABSTRACT FROM AUTHOR]