In this study, MnFe2O4/Fe3O4/PANI nanocomposites were synthesized via hydrothermal and coprecipitation methods and decorated on reduced graphene oxide (rGO) sheets with three weight ratios (1:1), (2:1), and (3:1) for MnFe2O4/Fe3O4/PANI versus rGO. FESEM images indicate a random distribution of MnFe2O4/Fe3O4 and PANI components on the rGO sheets. The designed superparamagnetic nanocomposites, MnFe2O4/Fe3O4/PANI/rGO, exhibit multi-reflections, strong interfacial polarizations, scattering of incident microwaves, and multiple magnetic resonances, which results in superior absorption performance. This is due to the structural design and distribution of different components providing various interfaces, high specific surface area, and different magnetic and dielectric components. The microwave absorption properties are evaluated in the frequency range of 1–18 GHz (L, S, C, X, and Ku bands), from electromagnetic parameters according to transmission line theory. Our results show that (MnFe2O4/Fe3O4/PANI)/rGO (1:1) presents the highest reflection loss, −108.71 dB, at 17.8 GHz with a thickness of 4.2 mm and bandwidth of 3.2 GHz. Interestingly, (MnFe2O4/Fe3O4/PANI)/rGO (3:1) shows a broad absorption bandwidth of 5.6 GHz for a thickness of only 2.2 mm, having a remarkable reflection loss of −95.52 dB at 17.8 GHz. Our study introduces a novel approach for the successful design and preparation of multi-dimensional graphene-based quaternary nanocomposites compromised from lightweight microwave absorbers, with numerous heterogeneous interfaces and defects resulting from interfacial engineering that have promising potential applications in broadband microwave absorption.