Chalcopyrites demonstrate compelling features for optoelectronic and photovoltaic devices, attributed to their valuable properties. Their remarkable light-absorption capabilities and well-suited band gap render them so attractive for applications in these fields. By allowing low-energy sub-bandgap photons to pass through and reducing the thermalisation loss from high-energy photons, intermediate-band materials address the primary problems in solar cells. This approach allows for more efficient use of the solar spectrum, helping solar cells exceed the traditional efficiency limits defined by the Shockley-Queisser limit. The objective of this study was to evaluate the electronic and optical characteristics of CuAlS2 systems doped with transition metals (TM = Mn, Fe) using the Full Potential Linearized Augmented Plane Wave approach within the framework of Density Functional Theory. A stable phase within the systems was observed upon replacing the Al atom with TM. The functionality of the intermediate band was governed by the 3d electronic characteristics of the TM3+ ion and its electronic configuration. The optical properties of CuAlS2 doped with Mn and Fe were analysed by calculating the dielectric function, refractive index, reflectivity, and absorption coefficient. Furthermore, the introduction of Mn and Fe through doping led to the creation of an intermediate band, enhancing visible light absorption and power conversion efficiency. Consequently, the optical spectrum of Mn-doped CuAlS2 and Fe-doped CuAlS2 compounds exhibits additional absorption peaks, accompanied by a significant improvement in absorption intensity. Our findings highlighted the need for continued and futuristic research into the scalability of these materials for practical applications in solar cells, optoelectronics, and spintronic devices. This investigation suggests that Mn-doped CuAlS2 holds the highest potential due to its high charge carriers and low recombination rate, indicating enhanced performance in CuAlS2-based intermediate band solar cells.