The ORCID identification number(s) for the author(s) of this article can be found under https://doi.org/10.1002/smll.202004579.heterogeneous catalysis has received more attention recently due to the merits of easy separation/recycling and achieving green reaction process. [3] Precious metals such as platinum, ruthenium, gold, and palladium are found to afford excellent catalytic activity for the selective oxidation of alcohols, [2a,4] however, their scarcity and high cost hinder the real applications for chemical industry. As an alternative, the catalysts based on earth-abundant transition metals are investigated to activate different oxidants including molecular oxygen, ozone, and liquid peroxides (i.e., hydrogen peroxide and tert-butylhydroperoxide) for oxidative applications. [5] The particle size and dispersion of the metal/ metal oxides play a pivotal role in affecting the catalytic performance. Therefore, much attention has been focused on reducing the particle size and optimizing the coordination between the metals and supports. Graphene based materials are extensively studied as substrate to support highly dispersed metal particles owing to the high surface area and excellent chemical/electrochemical properties. [6] Single-atom catalysts (SACs) consist of individual atoms dispersed on and/or bonded with the surface atoms of an appropriate support with high selectivity, catalytic activity and excellent atomic efficiency. [7] The catalysts with supported