Researchers are in continuous search of better strategies to minimize, if not prevent, the anthropogenic release of toxic heavy metals, such as Cu(II) and Pb(II), into drinking water resources and the natural environment. Herein, we report for the first time the low-temperature combustion synthesis of magnetic chitosan-manganese ferrite in the absence of toxic cross-linking agents and its removal of Cu(II) and Pb(II) from single-component metal solutions. The nonlinear Langmuir model best described the isotherm data, while the nonlinear pseudo-second order model best described the kinetic data, signifying monolayer Cu(II) or Pb(II) adsorption and chemisorption as the rate-determining step, respectively. Adsorption capacities by magnetic chitosan-manganese ferrite obtained for both metals were consistently higher than those by manganese ferrite, indicating that chitosan enhanced the performance of the magnetic adsorbent. The maximum adsorption capacities of magnetic chitosan-manganese ferrite for Cu(II) and Pb(II) were 14.86 and 15.36 mg g−1, while that of manganese ferrite were 2.59 and 13.52 mg g−1, respectively. Moreover, the adsorbents showed superior binding affinity and sorption for Pb(II) than Cu(II) owing to the stronger ability of the former to form inner-sphere complexes with manganese ferrite and magnetic chitosan-manganese ferrite. Finally, thermodynamic studies revealed that the uptake of either Pb(II) or Cu(II) by magnetic chitosan-manganese ferrite was spontaneous and endothermic. The as-prepared adsorbent was characterized for morphology, elemental composition, surface functional sites, and particle size using scanning electron microscopy, energy dispersive spectroscopy, Fourier transform infrared spectroscopy, and dynamic light scattering technique, respectively.