Microcrystalline graphite (MG)/zinc ferrite (ZFO) composites were prepared by a high-temperature ball milling method. The magnetic and microwave absorption properties of MG/ZFO composites were analyzed in the frequency range of 2.0–18.0 GHz. The results showed that MG has a favorable impact on the microwave absorption capacity of ZFO. The composites containing 10 wt% MG had a minimum reflection loss of −62.90 dB, which is almost a factor of 12 higher than for pure ZFO, and their effective absorption bandwidth (EAB, RL<−10 dB) covers frequency range of 5.84–7.92 GHz for a matching thickness of 3.9 mm, and for a matching thickness of 1.8 mm, the EAB covers frequency range of 12.87–17.70 GHz. A probable mechanism of microwave absorption for MG/ZFO composites is based on a synergistic combination of dielectric and magnetic losses. The attractive properties of prepared composites indicate that they are promising and competitive materials for use in microwave absorption.