Nanomaterials properties are deeply dependent on several features, being easily tuned according to its composition, shape, and dimensionality. Graphene, a two-dimensional (2D) material has outstanding properties that may be tailored by turning its shape to 3D conformations, similar to crumpled paper ball-like structures. Thus, some drawbacks related to graphene restacking could be avoided, besides enlightening a way to explore the properties of graphene-based materials. Herein, we synthesize crumpled graphene structures fully decorated by manganese ferrite (MnFe2O4) nanoparticles in one single step. The samples were produced using an aerosol-assisted capillary compression process and the crumpled paper-ball-like shape of the composites could be adjusted to incorporate increasing amounts of manganese ferrite nanoparticles. We explored two different applications for the obtained materials: as an electrochemical sensor for hydrogen peroxide, and electrochemical supercapacitors. As a proof-of-concept, we synthesized bare manganese ferrite and a composite of flat rGO:MnFe2O4, which assisted us to certify that the best performance is related to the synergistic effect between components, the ratio between them, and the proper shape of the composite.