The construction of special three-dimensional microstructure is becoming an extremely fascinating approach to upgrade the electromagnetic properties of carbon-based microwave absorption materials (MAMs) recently. Herein, we have demonstrated the successful fabrication of a series of carbon nanotubes (CNTs)@Ni/C foams (CNCFs) through two-step pyrolysis processes. It is found that the loading amount of CNTs has an obvious influence on modulating the electromagnetic diameters of CNCFs, and thus effectively tuning their microwave absorption properties. With the relative carbon content of 66.3 wt%, CNCFs-2 exhibits admirable microwave absorption performance, including the effective absorption bandwidth of 5.8 GHz with the absorber thickness of 1.8 mm and the maximum reflection loss intensity of −47.0 dB therein. Electromagnetic analysis reveals that the intrinsic attenuation ability, well-matched characteristic impedance, and multiple reflection effect synergistically work for the excellent reflection loss characteristics of CNCFs-2, which indicates rational microstructure design and appropriate chemical composition regulation are vitally important for the enhancement of microwave absorption performance. We believe these desirable microwave absorption properties can make CNCFs-2 eligible to be a very promising candidate for high-performance MAMs, and this research will provide some inspirations more or less for the development of more advanced carbon-based MAMs in the future.