In this study, the synthesis and characterization of heterostructured WS2/BiOBr and WS2/BiOCl nanosheets are discussed and their catalytic activity in the light-activated oxidative coupling of arylamines to create diarylimines is evaluated. The bismuth halide photocatalysts were synthesized by a modified surfactant-assisted aqueous route. The size, crystalline structure and composition of each material were characterized through applications of UV-vis diffuse reflective spectroscopy (DRS), Fourier-transform infrared spectroscopy (FT-IR), Brunauer-Emmet-Teller (BET) analysis, and X-ray diffraction (XRD). This approach produced nanocatalyst architecture with optimal photocatalytic activity in visible light-activated coupling reactions that allows for improved active sites and better rates of decomposition of organic pollutants. By developing photocatalysts that are more effective (in a controlled environment), they can be applied in contaminated waters or soils to break down these chemicals and reduce the harmful impact on the environment.