This Account reviews recent advances in the liquid exfoliation of defect-free graphene. Graphene, a single layer of carbon atoms arranged in a hexagonal lattice, has unique physical properties that make it highly desirable for various applications. However, the production of high-quality, large-scale graphene remains a challenge. Liquid exfoliation offers a promising method to produce defect-free graphene in large quantities by dispersing graphite in solvents that match the surface energy of graphene. This process involves sonication of graphite powder in a suitable solvent, which exfoliates the graphite into nanosheets that are stabilized by the solvent. The optimal solvent surface energy is around 68 mJ/m², and the process can be optimized to produce large quantities of defect-free graphene. Surfactants can also be used to stabilize exfoliated graphene in water, where the zeta potential of the surfactant-coated graphene nanosheets controls the dispersed concentration. Liquid exfoliated graphene can be used for a range of applications, including optical limiters, transparent conductors, and mechanical reinforcement for polymer-based composites. The technique has also been extended to exfoliate other layered compounds such as boron nitride and MoS₂. This liquid exfoliation technique can be applied to a wide range of materials and has the potential to be scaled up into an industrial process. The coming decade is expected to see an explosion in the applications involving liquid exfoliated two-dimensional materials.This Account reviews recent advances in the liquid exfoliation of defect-free graphene. Graphene, a single layer of carbon atoms arranged in a hexagonal lattice, has unique physical properties that make it highly desirable for various applications. However, the production of high-quality, large-scale graphene remains a challenge. Liquid exfoliation offers a promising method to produce defect-free graphene in large quantities by dispersing graphite in solvents that match the surface energy of graphene. This process involves sonication of graphite powder in a suitable solvent, which exfoliates the graphite into nanosheets that are stabilized by the solvent. The optimal solvent surface energy is around 68 mJ/m², and the process can be optimized to produce large quantities of defect-free graphene. Surfactants can also be used to stabilize exfoliated graphene in water, where the zeta potential of the surfactant-coated graphene nanosheets controls the dispersed concentration. Liquid exfoliated graphene can be used for a range of applications, including optical limiters, transparent conductors, and mechanical reinforcement for polymer-based composites. The technique has also been extended to exfoliate other layered compounds such as boron nitride and MoS₂. This liquid exfoliation technique can be applied to a wide range of materials and has the potential to be scaled up into an industrial process. The coming decade is expected to see an explosion in the applications involving liquid exfoliated two-dimensional materials.