Copper antimony sulfide (CuSbS2) is a promising candidate in photovoltaic and photodetector applications due to its excellent optoelectronic properties. Pulsed laser ablation in liquid (PLAL) is an environment friendly technique for producing nanoparticles of metals, semiconductors, ceramics etc. Here we report the synthesis of CuSbS2 nanoparticles by pulsed laser ablation in different liquid media using different wavelengths. The nanoparticles were synthesized in solvents such as acetone, methanol, ethanol, isopropanol and dimethyl formamide using 532 and 1064 nm output from a pulsed Nd:YAG laser (10 ns, 10 Hz). Their morphology, structure, crystalline phase, elemental composition and optical properties are examined using transmission electron spectroscopy (TEM), X-Ray diffraction (XRD), Raman spectroscopy, X-Ray photoelectron spectroscopy (XPS) and UV-Visible absorption spectroscopy. We used spray deposition for the fabrication of nanostructured CuSbS2 thin films from the laser ablated nanocolloids in isopropanol and integrated the films in a solar cell as absorber for the first time. CAS thin films were characterized using various techniques and they are incorporated in a photovoltaic structure of superstrate configuration: Glass/FTO/CdS/Sb2S3/CuSbS2.