An assessment is offered regarding the progress made, and the remaining challenges, in the field of carbocatalysis. The fundamental principles that govern the preparation and performance of sp2-hybridized carbon materials in heterogeneous catalysis have been known for decades, and the level of understanding of key issues-especially the importance of textural and ion-exchange prop-erties (i.e., surface area, pore size distribution, and proton transfer)-remains quite satisfactory. The opportunities for novel catalytic materials-especially graphene nanosheets and carbon nanotubes-are tremendous, especially when it comes to taking advantage of their structural order, such that electron transfer can be both better understood and controlled to enhance catalytic activity and selectivity.