High reflection loss and wide absorption bandwidth materials are in great demand to prevent electromagnetic pollution and military applications. The composites prepared by combining different components with good dielectric and magnetic losses are expected to achieve ideal absorbing performance. In this study, a composite of cobalt nanoparticles enveloped in nitrogen-doped bamboo-like carbon nanotubes (Co@N-CNTs) was prepared by one-step annealing the mixture of melamine and cobalt nitrate at 800 °C in a mixed atmosphere of hydrogen and argon. Co nanoparticles derived from the reaction between H2 and cobalt nitrate during the sintering process were used as catalysts to prompt the carbonization of melamine and the formation of the bamboo-shaped N-doped carbon nanotubes, thus forming the composite structure of bamboo-shaped N-doped carbon nanotubes encapsulated with Co nanoparticles. This Co@N-CNTs composite not only had an excellent dielectric loss and magnetic loss but also greatly improved its impedance matching, thus having good electromagnetic wave absorption performance. The coating made from the Co@N-CNTs composite had a maximum reflection loss (RL) of −35.89 dB at only 1.8 mm thickness at 14.1 GHz and possessed an effective absorption bandwidth of up to 4.91 GHz (12.35–17.26 GHz), suggesting it a high-performance and wide-absorption bandwidth composite material.