It becomes more and more important to develop high-performance microwave absorbers and solve the problem of electromagnetic wave pollution. However, design of the microwave absorbers with wider effective absorption bandwidth and less filler loading still faces serious challenges. In this work, Ti3C2Tx nanosheets modified by Fe nanochain were prepared by the facile electrostatic self-assembly method. The Ti3C2Tx/Fe nanochain (Ti3C2Tx/Fe NCs-2) hybrids exhibit remarkable microwave absorption properties with the optimal reflection loss of −38.8 dB by thickness of 1.9mm. The effective absorption bandwidth reaches 6.72 GHz with the filler loading of 15 wt%. Furthermore, the radar cross-section reduction performance for hybrids has been proved by using computer simulation technology. When theta is at 0◦, the Ti3C2Tx/Fe NCs-2 shows the optimal radar cross-section reduction value of 19.43 dB. These results suggest that the Ti3C2Tx/Fe nanochain hybrid is a superior microwave absorber for practical applications.