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Cu₂ZnSnS₄ (CZTS) is a promising semiconductor material for photovoltaic applications, with excellent optical and electronic properties while boasting a nontoxic, inexpensive, and abundant elemental composition. Previous high-quality CZTS thin films often required either vacuum-based deposition processes or the use of organic ligands/solvents for ink formulation, which are associated with various issues regarding performance or economic feasibility. To address these issues, an alternative method for depositing CZTS thin films using an aqueous-based nanoparticle suspension is demonstrated in this work. Nanoparticles of constituent binary sulfides (Cu_xS and ZnS) are stabilized in an ink using tin(IV)-based, metal chalcogenide complexes such as [Sn₂S₆]^4−. This research paper provides a systematic study of the nanoparticle synthesis and ink formulation via the enabling role of the tin chalcogenide complexing power, the deposition of high-quality CZTS thin films via spin coating and annealing under sulfur vapor atmosphere, their structural characterization in terms of nanocrystal phase, morphology, microstructure, and densification, and their resultant optoelectronic properties.