A novel approach was employed to load α-Fe₂O₃ and α-FeOOH onto sewage sludge biochar (SBC) with the purpose of efficient nickel (Ni) removal. A high Ni(II) adsorption capacity of 35.50 mg·g^-1 in 100 ppm Ni(II) solution with 10 mg modified sewage sludge biochar (MSBC) was achieved. The adsorption kinetic and isotherm were fitted well by the pseudo-second-order model and the Langmuir model, respectively. The optimal pH was found around a neutral pH of 7. The adsorption mechanisms of Ni(II) onto MSBC were described as the synergistic effects of electrostatic attraction, ion exchange, inner-sphere complexation and co-precipitation. The initial rapid adsorption phenomenon could be attributed to electrostatic attraction and ion exchange, and then inner-sphere complexation and co-precipitation acted as a crucial role in the following step. The remarkable performance of MSBC provides an effective waste utilization approach to simultaneous sewage sludge recycle and Ni removal from aqueous solution.