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ZnO/Ni3ZnC0.7/x% CNT (x = 0, 2, 5, 10) urchin-like structures have been synthesized using a facile method based on metal-organic frameworks (MOFs) and applied as the electromagnetic absorber. The results of the experiments demonstrate that the content of multi-wall carbon nanotubes (MWCNT) has a great influence on the absorbing performance of the hybrid material. Conduction loss, interfacial polarization and ferromagnetic resonance all contribute to the electromagnetic absorption. The urchin-like ZnO/Ni3ZnC0.7/5% CNT composite presents excellent absorbing properties. When the filler loading of ZnO/Ni3ZnC0.7/5% CNT composite in paraffin matrix is only 10 wt.%, a minimum reflection loss of −33.2 dB is achieved at a layer thickness of 4.9 mm.