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A new layered metal sulfide, namely (C6H15N3)1.3(NH4)1.5H1.5In3SnS8 (1, C6H15N3 = N-(2-aminoethyl) piperazine), has been solvothermally synthesized and characterized. Compound 1 crystallizes in the monoclinic space group C2/c. Its structure features a two-dimensional layer of {In3SnS8}n3n− with the (4,4) topology net, which is formed by interlinking supertetrahedral T2 clusters as secondary building units. Band structure calculations revealed that 1 had a band gap of 2.7 eV. The photoelectric response of 1 showed steady and reversible on/off cycles with an "on" state of 121.13 nA cm−2. Moreover, the activation of 1 by replacing the sluggish organic cations with harder K+ ions endowed the material with improved adsorption performances for Sr2+ ions from aqueous solutions. [ABSTRACT FROM AUTHOR]