A novel low-cost polyvinyl alcohol modified chitosan-mycelium (MCMP) biosorbent was prepared and used for Cu(II) removal from aqueous solutions. SEM, mercury intrusion, and FTIR were employed for characterization. The optimum pH for Cu(II) adsorption was 4-5. Kinetic study showed that Cu(II) adsorption on MCMP followed the pseudo second-order kinetic model. The equilibrium data at different temperatures were well fitted by the Langmuir isotherm. The thermodynamic study proved the spontaneous and endothermic nature of the chemisorption process. MCMP could be reused for 10 adsorption-desorption-regeneration cycles without significantly reducing its adsorption capacity. MCMP adsorption is an inexpensive and promising method for Cu(II) removal from dilute solutions.