Exploring high-performance electromagnetic wave (EMW) absorption materials holds extraordinary potential for new-generation wireless communication and integrated electronics. Herein, a series of heterogeneous hydrangea-like NiMn-layered double hydroxide (NiMn-LDH)/MXene (denoted as NMM) hybrids were successfully synthesized by facile hydrothermal method and followed electrostatic self-assembly strategy. The EMW absorption performance of NMM hybrids could be flexibly tuned by regulating the ratios of NiMn-LDH to MXene. Benefiting from the synergy of unique structural design and various EMW attenuation mechanisms, the resultant NMM hybrids realize excellent EMW absorption performance. The NMM3 hybrid (the ratio of NiMn-LDH to MXene is 1:1) achieves an optimal reflection loss of –47.7 dB at 13.29 GHz with a thickness of 1.68 mm and a broad effective absorption bandwidth of 4.4 GHz (13.6-18.0 GHz) at a tiny thickness of 1.43 mm. Moreover, the radar cross section simulation is used to intuitively reveal the effectiveness of NMM hybrids as high-performance EMW absorption materials in actual application. This work provides an innovative perspective on the controllable design of highly efficient EMW absorption materials with remarkably practical application value.