Noble metals (Au, Pt, and Ru) loaded into carbon supports show excellent performance for CO oxidation. Herein, a tunable metal-organic framework (MOF) coating is applied to a macroscopic 3D Ru/graphene aerogel (Ru/GA) composite, using a facial step-by-step method. The open macroporous structure of the Ru/GA provides pathways for the access and diffusion of reactant and product molecules. The resulting HK (HKUST-1)-containing MOF composite exhibits good performance for CO adsorption. It can simultaneously adsorb and oxidize CO, which improves the reaction rate. In this work, the catalytic efficiency of the resulting catalyst is higher than that (≈48.4%) of the Ru/GA. These findings provide a simple method for increasing the instantaneous concentration of reactants around the catalyst, which in turn increases the reaction rate. The catalytic performances of composites subjected to different pretreatment conditions are also investigated. Hopefully, this finding may provide a feasible direction for the effective management of the diverse environment issues.