The competency of mango leaf powder (MLP), an eco-friendly and cost-effective adsorbent, has been extensively studied for the removal of a carcinogenic azo dye, acid yellow-99 (AY-99), from simulated wastewater on principal interest in combating water pollution and to comprehend the mechanisms of the phenomenon. Optimum dye adsorption occurs at pH 2.5, whereas the temperature has no significant effect. MLP can effectively adsorb 708.15 mg g −1 of dye as a function of the initial dye concentration with excellent fitting to the Langmuir isotherm model illustrating monolayer adsorption. The process is rather swift to be completed within ~ 160 min following film diffusion model and pseudo-second-order rate kinetics. The magnitude of hindrance exerted by NaCl in dye adsorption is found to be quite insignificant. The biomass is competent enough for anionic dye decolourization in the binary mixture (AY-99 + AR-88) determined by the first-order derivative spectrophotometric method. Thermodynamically the process is spontaneous, endothermic and entropy-driven. Zeta potential, XRD, SEM-EDXA and X-ray elemental mapping analyses have been used to assess the morphological changes and the mechanisms of dye interaction with MLP. FTIR spectroscopy and chemical modification of functional groups of biomass establish the major contribution of hydroxyl groups for effective dye decolourization through complexation and electrostatic interactions.