This work provides a first pivotal stepping-stone to exploring the immense possibilities of the proposed nanostructures in future theoretical/experimental studies. All analyses considered, in addition to comparisons with related hybrid structures, show some interesting potential uses for Phos-Fullerene nanostructures. For instance, covalent Phos-Fullerene complexes display a graphene nanobud-like structure and strong electron transfer in the Phos→Fullerene direction. In this regard, graphene nanobuds have shown potential uses in energy and gas storage devices with high stability at room temperature, new spintronics, position sensing, and graphene band structure engineering . Furthermore, Li adsorption was enhanced for graphene-C60 nanobuds by the high electron affinity of C60 and the charge transfer from graphene to C60 . Accordingly, the strong charge transfer in the Phos→Fullerene direction turns covalent complexes into remarkable candidates to be studied as novel storage and anode materials in Li/Na-ion battery applications.