Activated sludge, which is difficult and expensive to treat and dispose of, is a key concern in wastewater treatment plants. In this study, magnetic sludge biochar containing activated sludge and different sizes (14.3, 40.2 and 90.5 nm) of Fe
3
O
4
nanoparticles was investigated as an effective adsorbent for tetracycline (TC) adsorption. Magnetic sludge-based biochar was prepared by a facile cross-linking method and characterized by transmission electron microscopy, Fourier transform infrared spectroscopy (FTIR), X-ray diffraction, X-ray photoelectron spectroscopy (XPS) and zeta potential analysis. The adsorption performances of TC on three kinds of adsorbents were investigated. Although 14.3 nm Fe
3
O
4
nanoparticles could be inclined to aggregate and partially filled with pores of biochar, it turned out that magnetic sludge biochar with 14.3 nm Fe
3
O
4
nanoparticles exhibited optimum performance for TC removal with adsorption capacity up to 184.5 mg g
−1
, due to the larger amounts of functional groups and the change of zeta potential. Furthermore, the adsorption kinetics of TC on three kinds of adsorbents were studied, which implied that the pseudo-second-order kinetic model exhibited the better fit for the entire sorption process.