Hierarchical structural design has been proved to be a new strategy for fabricating high-performance microwave absorbers, so some researchers use low–dimensional components to construct continuous networks for better performance. In this work, the novel hierarchical carbon [email protected]–[email protected]2 film with tunable and efficient electromagnetic wave (EMW) absorption performance was obtained by the electrostatic spinning of ZIF–67 in the interior of carbon fibers and subsequent hydrothermal of MoS2. By the synergistic effects from the ZIF–67 particles increasing the magnetic loss and MoS2 at the outer layer improving the impendence matching, the absorption property of CPZM–1 could be summarized as follow: the optimal reflection loss(RL) was −72.7 dB with a thickness of 2.6 mm at 10.0 GHz and the corresponding effective absorption bandwidth (EAB) of 9.8 GHz covered whole X and Ku band. Moreover, by adjusting the load of ZIF–67, CPZM–5 achieved the maximum EAB of 12.5 GHz.