A nanoporous and large surface area (∼800 m ²/g) graphene-based material was produced by plasma treatment of natural flake graphite and was subsequently surface decorated with platinum (Pt) nano-sized particles via thermal reduction of a Pt precursor (chloroplatinic acid). The carbon-metal nanocomposite showed a ∼2 wt% loading of well-dispersed Pt nanoparticles (<2 nm) across its porous graphene surface, while neither a significant surface chemistry alteration nor a pore structure degradation was observed due to the Pt decoration procedure. The presence of Pt seems to slightly promote the hydrogen sorption behavior at room temperature with respect to the pure graphene, thus implying the rise of “weak” chemisorption phenomena, including a potential hydrogen “spillover” effect. The findings of this experimental study provide insights for the development of novel graphene-based nanocomposites for hydrogen storage applications at ambient conditions.