In this study, we developed a novel nanocomposite, polyurethane foam impregnated with zero-valent iron nanoparticles (PU@nZVI), for the effective removal of chromium(VI) from various water sources. The characterization of nanocomposite (PU@nZVI) was performed by XRD, SEM–EDS, TEM and FT-IR techniques. Using the response surface methodology, we optimized the removal conditions, achieving an optimal pH of 2 and a dose of 0.5 g/L. The PU@nZVI demonstrated an excellent maximum adsorption capacity of 600.0 mg/g for Cr6+. The adsorption kinetics and isotherms were best described by the pseudo-second-order model and the Freundlich isotherm, respectively. Significantly, the nanocomposite removed 99.98% of Cr6+ from tap water, 96.81% from industrial effluent, and 94.57% from treated sewage wastewater. Furthermore, the PU@nZVI maintained its efficiency over five adsorption–desorption cycles, highlighting its reusability. These results suggest that the PU@nZVI nanocomposite is a highly efficient and sustainable option for chromium(VI) removal in water treatment applications.