Carbon catalysis is an attractive metal-free catalytic transformation, and its performance is significantly dependent on the number of accessible active sites. However, owing to the inherent stability of the C–C linkage, only limited active sites at the edge defects of the basal plane can be obtained even after a harsh oxidation treatment. Therefore, to promote the development of carbocatalysis, it is highly desirable to enhance the density of the intrinsic active sites of carbon from the perspective of the methodology.