Carbon-based materials have demonstrated remarkable potential in heterogeneous catalysis for chemical synthesis, energy conversion, and environmental remediation, owing to their tunable structural properties. In this review, we summarize recent progress in carbon materials optimizing catalytic performance mainly from three aspects: (i) modulation of the geometric and electronic structures of active metal sites through tuning metal-support interactions; (ii) regulation of molecular sorption behaviors during catalysis; and (iii) the synergistic interplay between these two factors, which enables cooperative enhancement of catalytic performance. The wettability of carbon materials can be precisely modulated to facilitate mass transport of reactants and/or products on the catalyst surface, thereby enhancing catalytic performance. In addition, the abundant defect sites and well-developed pore structures of carbon materials can precisely regulate the spatial distribution of metal species and significantly improve their sintering resistance. These insights are expected to offer valuable design principles for the development of highly efficient carbon-based materials for thermocatalytic applications.