In this study, we have grown CuxSb1-xS2 (x = 0.2, 0.4, 0.6, 0.8) crystals using Bridgman technique by varying compositions of Cu and Sb and explored the impact on its structural, optical, thermal and electrical properties compared to pure CuSbS2. X-ray diffraction analysis confirmed the orthorhombic CuSbS2 phase and secondary phases due to different compositions of Cu and Sb. Stoichiometry of each crystal was verified through Energy dispersive X-ray analysis and uniform distribution was observed in elemental mapping. Field emission microscopy in scanning mode validated the flat surface and layer growth mechanism of all crystals. Raman spectroscopic measurements indicated the presence of Ag vibration modes with red shift in all crystals. The direct bandgap of CuxSb1-xS2 (x = 0.2, 0.4, 0.6, 0.8) crystals reduces from 1.65 eV to 1.61 eV with increasing Cu content which is determined using Kubelka-Munk function. These suitable bandgaps positioned them as promising candidates for optoelectronic applications. All four crystals were identified as p-type semiconductors based on variations in Seebeck coefficient (S), dc electrical conductivity (σ), and thermal conductivity (κ) within the temperature range of 313 K–573 K. Analysis of temperature-dependent variations in the power factor (S2σ) and figure of merit (ZT) highlighted the superior performance of Cu0.4Sb0.6S2 crystal compared to other grown crystals, reaching a maximum ZT value of 0.038 at 573 K. Thermogravimetric profiles conducted under nitrogen (N2) atmosphere revealed two-step decomposition for all crystals, with Cu0.4Sb0.6S2 experiencing the highest weight loss of 9.55 % and Cu0.8Sb0.2S2 displaying the lowest weight loss of 2.46%. Room temperature I–V characteristics and pulse photoresponse of prepared CuxSb1-xS2 (x = 0.2, 0.4, 0.6, 0.8) crystals photodetectors were measured for parallel to plane configuration, revealing that Cu0.6Sb0.4S2 exhibited the highest responsivity and detectivity of 32.718 μ A/W and 15.267 × 106 Jones, respectively.