Three new indium sulfides, [Ni(dien)2]0.5[InS2] (dien = diethylenetriamine) (1), [Ni(dap)3]0.5[InS2] (dap = 1,2-diaminopropane) (2), and [Ni(tepa)]2[In4S7(SH)2].H2O (tepa = tetraethylenepentamine) (3), have been prepared under solvothermal conditions and characterized by single-crystal X-ray diffraction. Compounds 1 and 2 consist of discrete 1-D {[InS2]-} infinity chains with complex cations as charge-compensating ions, while compound 3 consists of a novel 1-D anionic chain constructed from arachno-shaped In4S11 clusters. The sulfide chain of 3 coordinates into the complex cations via the nonterminal S atoms of the polymeric anion, forming a covalently linked organic-inorganic hybrid compound.