Accessibility of adequate safe and fresh water for human consumption is one of the most significant issues throughout the world and extensive research is being undertaken to resolve it. Nanotechnology is now an outstanding medium for water treatment and remediation from microorganisms and organic dyes, as compared to conventional treatment methods. For this task graphitic carbon nitride (g-C3N4) is a potential nanomaterial for environmental remediation, but its photogenerated charge carrier recombination rate restricts its use in practical applications. Hence, in the current study, we used a simple one-step calcination method to synthesize various ratios of ZnO/g-C3N4 binary nanocomposites. The band gap of g-C3N4 is 2.70 eV, but it is shifted to 2.60 eV by the 0.75 : 1 ZnO/g-C3N4 binary nanocomposite. Moreover, phase structure, morphology, thermal stability, oxidation state, elemental analysis, and surface area were evaluated using XRD, SEM, TEM, TGA, XPS, and BET analysis. The optimal ZnO loading content was determined and the mechanism of enhanced photocatalytic activity was studied in detail. The photocatalytic efficiency of the best catalyst was employed for the degradation of textile effluent followed by phytotoxicity evaluation using methylene blue (MB), and rhodamine B (RhB) as a model substrate was tested. Furthermore, the textile effluent treatment analysis discovered that the 75 mg concentration of 0.75 : 1 ZnO/g-C3N4 catalyst degraded up to 80% within 120 min and significantly reduced the concentrations of different physico-chemical parameters of textile effluents. These treated effluents have no phytotoxic effects on fenugreek plants, according to a pot study. It was found that the mesoporous 0.75 : 1 ZnO/g-C3N4 catalyst can be used as an effective and low-cost technique for the degradation of azo dyes in textile wastewaters.