In the past decades, remarkable progress has been achieved in the exploration of electrocatalysts with high activity, long durability, and low cost. Among these, defective graphene (DG)-based catalysts are considered as one of the most potential substitutes for precious metal-based electrocatalysts. DG-based catalysts contain abundant active centers with different configurations resulting from their extraordinary high-structural tunability. Herein, an overview on recent advancements in developing four kinds of DG-based catalysts is presented: 1) heteroatoms-doped graphene; 2) intrinsic DG (vacancy and topological defect); 3) nonmetal atoms or/and metal species-modified intrinsic DG (heterogeneous species and intrinsic defects co-tuned DG); and 4) DG-based van der Waals-type multilayered heterostructures. In particular, the synergistic effects between various defects are discussed, and the origin of catalytic activity is reviewed. Meanwhile, the established defect-derived catalytic mech
Two-dimensional (2D) layered materials have been widely used as catalysts due to their high specific surface area, large fraction of uncoordinated surface atoms, and high charge carrier mobility. Moiré superlattice emerges in 2D layered materials with twist angle or lattice mismatch. By manipulating the moiré superlattice structure, 2D layered materials present modulated electronic band structure, topological edge states, and unconventional superconductivity which are tightly associated with the performance of catalysts. Hence, engineering moiré superlattice structures are proposed to be an important technology in modifying 2D layered materials for improved catalytic properties. However, currently, the investigation of moiré superlattice structure in a catalytic application is still in its infancy. This perspective starts with the discussion of structural features and fabrication strategy of 2D materials with moiré superlattice structure. Afterward, the catalytic applications, inc