generation efficiency by reducing heat loss to the bulk water as well as the environment. [22][23][24] As such, efforts have been made in finding the optimal materials with excellent photothermal conversion and heat localization functions, such as plasmonic metals and semiconductors. [25][26][27][28][29][30][31] Among all the possible candidates, carbon materials demonstrate competitive merits due to their intrinsic high solar absorption, excellent structural tunability, and great processability to fulfill the demanding requirements in interfacial SVG. Carbon materials, especially graphene family, carbon nanotubes, and amorphous carbon composed of graphite carbon, can intrinsically convert solar flux into thermal energy by the excitation-relaxation process, conjugating electrons in unsaturated bonds, which lays the foundation for functioning as solar absorbers. [32] Furthermore, the tunable structures of carbon materials confer various functional properties to the system. The solar absorption ability can be enhanced by tailoring carbon nanotubes into vertically aligned arrays, enabling broad-spectrum absorption by multiply reflections in elongated light paths. [33] The 3D carbon monoliths, such as carbon foam and aerogel, can achieve capillary water uptake and thermal insulation, wherein the interconnected pore structure plays a dominating role in these processes. [34][35][36] More importantly, carbon materials, with great processability in different treatment approaches, can serve as ingredients coupling with other materials to form structured composites, achieving cooperative functionalities beyond individuals. For instance, graphene can be grown on the metal skeleton by chemical vapor deposition (CVD) method, endowing the system with more developed pore structures; 3D printing can fabricate patterned architecture on the chosen matrix, propitious to the interfacial water/thermal behavior regulation. [36,37] Meanwhile, the high natural abundance of carbon materials leads to its easy accessibility, which outperforms other materials. With those attractive advantages, carbon materials are capable of advancing interfacial SVG. [38] In this Review, we systematically summarize the design principles and recent progress of carbon materials in interfacial SVG technology (Figure 1). The parallelism between carbon materials structures and required functions for interfacial SVG is discussed. We then examine the recent progress on different interfacial SVG systems composed of artificial carbon materials (pristine carbon system and carbon-containing composite) and biochar, with the focus on the structure-property relationship. Several strategies for antisalt-fouling in the SVG desalination systems are elaborated. Finally, we underline the remaining challenges and provide perspective directions for future investigations.Seawater desalination is viewed as a promising solution to world freshwater scarcity. Solar assisted desalination is proposed to overcome the high energy consumption in current desalination technologies, as it ...