Artificial photosynthesis harnesses clean and sustainable solar power to catalyze the conversion of CO2 and H2O molecules into valuable chemicals and O2. This sustainable approach combines energy conversion with environmental pollution control. Non-oxide photocatalysts with broad visible-light absorption and suitable band structures, hold immense potential for CO2 conversion. Nevertheless, they still face numerous challenges in practical applications, particularly in CO2 conversion with H2O. Surface modification and functionalization play the significant role in improving the activity of non-oxide photocatalysts. Multifarious strategies, such as cocatalyst loading, surface regulation, doping engineering, and heterostructure construction, have been explored to optimize light harvesting, bandgap driving force, electron–hole pairs separation/transfer, CO2 adsorption, activation, and catalysis processes. This review summarizes recent progress in surface modification strategies for non-oxide photocatalysts and discusses their enhancement mechanisms for efficient CO2 conversion. These insights are expected to guide the design of high-performance non-oxide photocatalyst systems.