To achieve compact and light-weighted power conversion devices, magnetic core materials such as MnZn ferrite are highly desired with low core losses at high frequency above megahertz. In this work, high-valent Sn4+ ions were doped into the MnZn ferrite to manipulate the electromagnetic properties and suppress the high-frequency core losses. The distribution of Sn4+ in MnZn ferrite was investigated by TEM with energy dispersive X-ray analysis, which indicated that most of the substituted Sn4+ ions remained at the grain boundaries rather than dissolving into the lattice, and thus greatly impacted the electromagnetic properties of MnZn ferrite. The initial permeability and saturation induction decreased with the Sn substitution monotonically. The core loss was reduced to 457 kW/m3 at 3 MHz, 30 mT, and 25oC when the Sn substitution content was 0.003, due to the effective suppression of eddy current loss and residual loss. The sample with Sn content of 0.003 exhibited excellent overall electromagnetic properties, which could be potentially useful in high-frequency transformers, converters, and power sources.