Sugarcane bagasse biosorbents were tested for biosorption of phenol and cyanide from synthetic/simulated wastewater. The influence of pH, biosorbent dose, temperature, contact time, and initial concentration of phenol and cyanide was investigated. At an optimum temperature 30°C, pH 7, and the biosorbent dose of 40 g/L, 66.78% phenol and 79.30% cyanide were removed from binary aqueous solution containing 300 mg/L of phenol and 30 mg/L of cyanide. The equilibrium state was achieved after about 34 and 32 h, respectively, for phenol and cyanide at a temperature of 30°C. The extended Freundlich model fits the binary equilibrium data suitably for both phenol and cyanide. The kinetic modeling results showed that fractal-like models and BrouserWeron-Sototlongo for phenol and cyanide were capable to provide realistic explanation of biosorption kinetic. Biosorption of phenol and cyanide followed pseudo-secondorder kinetics, indicating chemisorption to be the mechanism of biosorption. The present study provides a new insight for the removal of phenol and cyanide onto sugarcane bagasse.