The enhancement of thermally conductive performances for lightweight thermal interface materials is a long-term effort. The superb micro-structures of the thermal conductivity enhancer have an important impact on increasing thermal conductivity and decreasing thermal resistance. Here, globular flower-like reduced graphene oxide (GFRGO) is designed by the self-assembly of reduced graphene oxide (RGO) sheets, under the assistance of a binder via the spray-assisted method for silicone-based spherical alumina (S-Al2O3) composites. When the total filler content is fixed at 84 wt%, silicone-based S-Al2O3 composites with 1 wt% of GFRGO exhibit a much more significant increase in thermal conductivity, reduction in thermal resistance and reinforcement in thermal management capability than that of without graphene. Meanwhile, GFRGO is obviously superior to that of their RGO counterparts. Compared with RGO sheets, GFRGO spheres which are well-distributed between the S-Al2O3 fillers and well-dispersed in the matrix can build three-dimensional and isotropic thermally conductive networks more effectively with S-Al2O3 in the matrix, and this minimizes the thermal boundary resistance among components, owning to its structural characteristics. As with RGO, the introduction of GFRGO is helpful when decreasing the density of silicone-based S-Al2O3 composites. These attractive results suggest that the strategy opens new opportunities for fabricating practical, high-performance and light-weight filler-type thermal interface materials.