Metal-organic frameworks (MOFs) have drawn a lot of interest as prospective starting points for highly effective electromagnetic wave (EMW) absorbers. However, the inevitable shrinkage and probable densification that occur during pyrolysis significantly reduce the microwave-loss capacity. A dual-layer MOF, ZIF-8@ZIF-67, is created and effectively decorated on graphene sheets as a solution to this problem. The shrinkage and densification were then suppressed by the subsequent pulverization effect between the two MOFs. Due to suitable compositions and specialized microstructures, G/Co@C exhibits excellent impedance matching and dissipates EMW by combining magnetic and dielectric loss. The maximum reflection loss of G/Co@C-7/paraffin is -55.0 dB at 5.8 GHz with just 7% filler. Therefore, the preparation of high-efficiency MOF-derived microwave absorbers by the pulverization effect is demonstrated to be an efficient strategy.