Single‐atom catalysts (SAC) can boost the intrinsic catalytic activity of hydrogen evolution reaction (HER) and oxygen reduction reaction (ORR). However, the challenge remains due to the complex synthesis process and insufficient stability. A sustainable approach is applied to synthesizing SACs through laser irradiation and gaining mesoporous graphene oxide (MGO). The surface dangling bonds of nitrogen‐doped MGO (NMGO) extract metal atoms species from Co or Fe metal foams and convert them to SAC via an appropriate synthesis approach. Notably, the Co‐NMGO electrocatalyst requires low potentials of 146 mV to convey a current density of 10 mA cm−2 towards HER. Similarly, the Fe‐NMGO electrocatalyst offers an onset of 0.79 V towards ORR in acidic solution. The individual metal atoms are confirmed via aberration‐corrected scanning transmission electron microscopy, and X‐ray absorption near‐edge structure and extended X‐ray absorption fine structure. Density functional theory calculations by applying the grand canonical potential kinetics model revealed that Co‐NMGO shows the optimum free reaction energy of −0.17 eV at −0.1 V for HER, and Fe‐NMGO has less limiting potential than that of Co‐NMGO for ORR case. This work opens a new approach towards the synthesis of SAC and its mechanistic understandings.

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