Cobalt sulfide composites have exhibited great potential in terms of microwave absorption, owing to their low price, relatively high capacitance, and excellent electrocatalytic activity. Thus, a novel core-shell like structure comprising cobalt sulfide@polypyrrole (CoS@PPy) composite was synthesized by a facile solvothermal synthesis method and in situ polymerization. When coated by the heterostructure polypyrrole aerogel, CoS@PPy composite exhibited excellent microwave absorption properties with an optimal reflection loss (R_L) of −41.8 dB at 6.96 GHz. Furthermore, the absorption bandwidth (R_L < −10 dB) of 5.4 GHz could be reached at a coating thickness of 2.05 mm, probably attributing to the synergistic effect of good impedance matching, interfacial polarization, dipole polarization, and conductivity loss. Moreover, this work proposed a loss mechanism mode which probably occurred in the CoS@PPy composites. It was demonstrated that the CoS@PPy composite is a promising material in the field of electromagnetic wave absorption.