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In this work, a nanocomposite consisting of ternary chalcogenide CuInS₂ and TiO₂ was prepared and its optical and optoelectrical properties were investigated. The CuInS₂/TiO₂ nanocomposite was produced via one-step mechanochemical synthesis and characterized from the crystal structure, microstructural, morphology, surface, optical, and optoelectrical properties viewpoints. X-ray diffraction confirmed the presence of both components, CuInS₂ and TiO₂, in the nanocomposite and revealed a partial transformation of anatase to rutile. The presence of both components in the samples was also proven by Raman spectroscopy. HRTEM confirmed the nanocrystalline character of the samples as crystallites ranging from around 10 nm and up to a few tens of nanometers were found. The presence of the agglomerated nanoparticles into larger grains was proven by SEM. The measured optical properties of CuInS₂, TiO₂, and CuInS₂/TiO₂ nanocomposites demonstrate optical bandgaps of ~1.62 eV for CuInS₂ and 3.26 eV for TiO₂. The measurement of the optoelectrical properties showed that the presence of TiO₂ in the CuInS₂/TiO₂ nanocomposite increased its conductivity and modified the photosensitivity depending on the ratio of the components. This study has demonstrated the possibility of preparing a CuInS₂/TiO₂ nanocomposite material with promising applications in optoelectronics in the visible region in an eco-friendly manner.