Correlated electronic materials (CEMs) with strong electron−electron interactions are often associated with exotic properties, such as metal‐insulator transition (MIT), charge density wave (CDW), superconductivity, and magnetoresistance (MR), which are fundamental to next generation condensed matter research and electronic devices. When the dimension of CEMs decreases, exposing extremely high specific surface area and enhancing electronic correlation, the surface states are equally important to the bulk phase. Therefore, surface/interface chemical interactions provide an alternative route to regulate the intrinsic properties of low‐dimensional CEMs. Here, recent achievements in surface/interface chemistry engineering of low‐dimensional CEMs are reviewed, using surface modification, molecule−solid interaction, and interface electronic coupling, toward modulation of conducting solids, phase transitions including MIT, CDW, superconductivity, and magnetism transition, as well as external‐field response. Surface/interface chemistry engineering provides a promising strategy for exploring novel properties and functional applications in low‐dimensional CEMs. Finally, the current challenge and outlook of the surface/interface engineering are also pointed out for future research development.