Manganese-zinc (MnZn) ferrites have important applications in energy conversion, transmission, and harvesting. MnZn ferrite for magnetic field energy harvesting is expected to enhance the saturation magnetic induction (Bs), initial permeability (μi), and Curie temperature (Tc) aspects simultaneously, which is beneficial to the energy harvesting efficiency and safety of the device. In this paper, various formulations of MnZn ferrite samples were prepared by the conventional oxide ceramic process. The cation distribution was determined through Rietveld refinement of XRD patterns Based on this, the M–T curves were fitted by combining Néel molecular field theory with Brillouin functions. The greatest influence on the Curie temperature was found to be the molecular field coefficient between the A and B sites. The magnetization mechanism of MnZn ferrite was comprehensively analyzed by fitting the complex permeability spectrum, magnetocrystalline anisotropy constant, and magnetostriction coefficient. The ratio of domain wall displacement magnetization to domain rotation magnetization shows an increasing and then decreasing trend with Fe content, while |K1| shows an opposite trend. Finally, MnZn ferrite materials with excellent overall performance (Bs = 505mT, μi = 9016, Tc = 447 K) were prepared by investigating the magnetization mechanism.