BiOCl/WO3 microcomposites were synthesized using a one-step hydrothermal route in the presence of a variety of surfactants: polyvinylpyrrolidone (PVP), triethylene glycol (TEG), and Triton X-100 (TX-100). The as-synthesized microcomposites were exploited as efficient adsorbents for removing organic dyes (rhodamine B and methylene blue). Prior to adsorption studies, the structural, functional, and morphological characteristics of these adsorbents were studied using analytical techniques, including XRD, FE-SEM, TEM, and UV-DRS, which revealed the presence of large surface areas. The experimental results show that the PVP-synthesized BiOCl/WO3 microcomposite was significantly more effective as an adsorbent than the microcomposites synthesized using TEG or TX-100. This enhanced adsorption performance is attributable to the larger surface area associated with the developed microstructure of the PVP-stabilized BiOCl/WO3 microcomposite. The BiOCl/WO3 microcomposite synthesized from PVP was subjected to parametric studies involving catalyst dosage, pH, and initial dye concentration. The experimental data were fitted to isotherm models, and the mechanism of adsorption was investigated.