The unregulated industrializations has poses serious threat to entire ecosystem by releasing untreated effluents containing hazardous dyes to fresh water. In the forefront polycationic ferrite (ternary ferrite)-chitosan microspheres were used to address the issue of synthetic dyes, contaminating water bodies. In the current study, visible light assisted ternary ferrite Fe2Ni0.5Cu0.5O4 (CNF-NPs) photocatalyst along with their binary ferrite photocatalysts Fe2CuO4 (CF-NPs) and Fe2NiO4 (NF-NPs) were prepared by a facile approach to compare the efficiency of ternary and binary ferrites photocatalysts for degradation of dye. Additionally, chitosan was used to support ferrites, and different chitosan-supported ternary ferrite microspheres (CNF-CM) and binary ferrite microspheres (CF-CM and NF-CM), were tailored respectively. FTIR analysis of CNF-CM composites shows presence of all the characteristics peaks of chitosan and CNF NPs confirming its synthesis. The calculated average crystallite size (18 nm) were obtained from Scherrer's equation applied to XRD data. The composition of CNF-NPs was confirmed by EDX analysis. The CNF-CM has 860 μm microsphere size with a smooth surface as shown in SEM images. The calculated optical band gap of the synthesized photocattalyst lies in visible region (2.01) obtained from Tauc’s plot. The photocatalyst CNF-CM showed 93% degradation efficiency for hazardous methylene blue (MB) and 90% efficiency for rhodamine b (RB) dyes within 140 min of sunlight irradiation at optimum conditions. Inorder to validate the photocatalytic efficiency of the CNF-CM, the experimental conditions were also optimized by statistical optimization methods (RSM, ANN). The ANOVA adequate precision (AP) value of 17.83 (> 4) for MB and 16.91 for RB suggests that the projected output variable range is relatively larger compared to the average standard error, further affirming the competence of the quadratic model.