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Heterointerface engineering is an attractive approach to modulating electromagnetic (EM) parameters and EM wave absorption performance. However, the weak interfacial interactions and poor impedance matching would lead to unsatisfactory EM absorption performance due to the limitation of the construction materials and design strategies. Herein, multilevel heterointerface engineering is proposed by in situ growing nanosheet-like NiCoO 2 and selenides with abundant interface structures on 3D-printed graphene aerogel (GA) skeletons, which strengthens the interfacial effect and improves the dielectric polarization loss. Benefiting from the features of substantially enhanced polarization loss and optimized impedance matching, the graphene/S-NiCoO 2 /selenides (G/S-NCO/Se) have achieved brilliant EM wave absorption performance with a strong reflection loss (RL) value of -60.7 dB and a broad effective absorption bandwidth (EAB) of 8 GHz, which is about six times greater than that of the graphene aerogel (-9.8 dB). Moreover, it is further confirmed by charge density differences and off-axis electron holography that a large amount of polarized charge accumulates at the interface, leading to significant polarization relaxation behaviors. This work provides a deep understanding of the effect of a multilevel heterogeneous interface on dielectric polarization loss, which injects a fresh and infinite vitality for designing high-efficiency EM wave absorbers.