Graphene (GR) is a flat monolayer of sp²-bonded single carbon atoms densely packed into a honeycomb crystal lattice. Due to its unique characteristics, GR is expected to contribute to enhanced nanoelectronic, bio-electronic devices, etc. in the near future. However, the single-layered GR sheets have a tendency to form irreversible aggregates or even to restack easily due to strong attraction between sheets. Preventing of aggregation and restacking of GR is achieved by the dimensional transition from flat sheets to fractal-dimensional, nearly spherical crumpled balls using aerosol spray pyrolysis. This review first introduces the fabrication of crumpled GR and GR-composite by aerosol spray pyrolysis, and then discusses the material properties of GR: strain-hardening, compression and aggregation-resistant behavior. Finally, we introduce effective applications of hollow crumpled GR balls for oil absorbent and crumpled GR-composites for glucose biosensor, respectively.