The present invention relates to a manufactured graphene/metal or metalloid core-shell composite and manufacturing method thereof. The method comprising: using a modified graphene oxide as a base, then performing concentration and steam drying followed by organic solvent replacement to obtain a modified graphene oxide organic solvent; using a liquid-phase self-assembly method to coat the modified graphene oxide onto a surface of the metal or metalloid to form a graphene/metal or metalloid coated particle solution, then filtering and drying to obtain the graphene metal/metalloid core-shell composite. The method improves upon a conventional organic and inorganic material coating technique, and reduces an impact of a water-based solvent and high temperature on a highly reactive metal and metalloid, thereby expanding the feasibility of the coating technique and addressing a barrier of applicability of graphene and reactive metal or metalloid in the field of energetic materials.