Discharging heavy metals into water bodies presents a serious environmental risk. Hexavalent chromium (Cr(VI)) is one of the harmful substances that pose substantial health hazards to humans. The aim of this research is to synthesize an organic composite photocatalyst by polymerizing m-phenylenediamine (mPD) and Terephthalic acid (TA) at high temperatures. TA and mPD interact and result in the formation of a polymerized-mPD-TA photocatalyst to reduce Cr(VI) under visible light. Field Emission Scanning Electron Microscopic (FESEM), Energy-Dispersive X-ray (EDX), Dynamic Light Scattering (DLS), Fourier-transform Infrared spectroscopic (FT-IR), Brunauer-Emmett-Teller (BET), UV–Vis Diffuse Reflectance Spectra (UV-vis-DRS), Electrochemical Impedance Spectroscopy (EIS) and Mott-Schottky methods were used to characterize the produced photocatalyst. The effect of operational parameters including pH, volume of hole scavenger, photocatalyst mass, and Cr(VI) initial concentration was investigated, and the optimum conditions were clarified. To investigate the adsorptive characteristics of the prepared photocatalyst, Isotherm, and Kinetic investigations were carried out. The adsorption studies revealed that the Freundlich and pseudo-second-order (PSO) models offered a better suitable match to the experimental data. In order to investigate the practicality of the photocatalyst, reusability, and sunlight tests were carried out, and it was shown that the prepared composite possessed great durability and could perform under sunlight to reduce Cr(VI).