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Design and fabrication of structurally optimized microwave absorbing materials are important for eliminating electromagnetic (EM) pollution. Herein, we reported the novel highly regulated core/shell bamboo-like polypyrrole (PPy) nanofibers/Fe3O4 hybrids as the efficient microwave absorbing materials. Typically, the target hybrid materials were prepared by a two-step method, including synthesis of bamboo-like PPy nanofibers using vapor polymerization of PPy on tubular vanadium pentoxide templates and coprecipitation of Fe3O4 nanoparticles on the surface of bamboo-like PPy nanofibers. Owing to good impedance matching and hierarchical structure, as-prepared core/shell bamboo-like PPy nanofibers/Fe3O4 hybrids exhibit superior microwave absorption and broad absorption bandwidths compared with conventional PPy/Fe3O4 composites. The lowest reflection loss of core/shell bamboo-like PPy nanofibers/Fe3O4 hybrid is calculated to be −41.6 dB at 10.0 GHz with the thickness of 2.5 mm. Furthermore, the absorption bandwidths exceeding −10 dB are more than 8.0 GHz with thickness of 2.0–3.5 mm. Therefore, this work provides an efficient way to obtain high-performance microwave absorber with lightweight, strong absorption and wide absorption bandwidths. [ABSTRACT FROM AUTHOR]