An ultralight Ni-MOF-rGO aerogel which possess the merits of not only broad bandwidth and strong absorption but also lightweight and thin matching thickness is fabricated through a hydrothermal treatment, freeze-drying, and annealing procedure. The Ni@C microspheres are dispersed randomly and evenly on the graphene oxide (GO) nanosheets, which can be proved through SEM and TEM results. The electromagnetic parameters of the composite can be adjusted by changing the mass ratio of the MOF and GO to endow the material with both good impedance matching and superior electromagnetic wave absorption performances. Consequently, the resulting composite shows outstanding microwave absorption performance, which achieves strong absorption (−51.19 dB) and broad effective absorption bandwidth (6.32 GHz) with a thickness of 1.9 mm while the filling content is only 2 wt %. In addition, the multiple loss mechanisms of the Ni-MOF-rGO aerogel are illustrated, including conduction loss, dipolar polarization, interfacial polarization, magnetic resonance, and eddy current loss. In a word, the extraordinary microwave absorption performance is ascribed to the synergistic effects of the unique multiple layered structure of GO and the hollow core−shell structure of the Ni@C microsphere. This work demonstrates that the ultralight aerogel with excellent electromagnetic wave absorption performance is a promising strategy for microwave absorption application.