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In this study, we report the optoelectric and thermoelectric properties of famatinite Cu₃SbS₄ that was mechanochemically synthesized in a planetary mill from powder elements for 120 min in an inert atmosphere. The tetragonal famatinite Cu₃SbS₄ was nanocrystalline with a crystallite size of 14 nm, as endorsed by Rietveld refinement. High-resolution transmission electron microscopy showed several crystallites in the range of 20–50 nm. Raman spectroscopy proved the purity of the synthesized famatinite Cu₃SbS₄ and chemical-state characterization performed by X-ray photoelectron spectroscopy confirmed that the prepared sample was pure. The Cu¹⁺, Sb⁵⁺, and S²⁻ oxidation states in Cu₃SbS₄ sample were approved. The morphology characterization showed homogeneity of the prepared sample. The photoresponse of Cu₃SbS₄ was confirmed from I–V measurements in the dark and under illumination. The photocurrent increase reached 20% compared to the current in the dark at a voltage of 5 V. The achieved results confirm that synthesized famatinite Cu₃SbS₄ can be applied as a suitable absorbent material in solar cells. The performed thermoelectric measurements revealed a figure of merit <i>ZT</i> of 0.05 at 600 K.