The article discusses the importance of surface engineering in enhancing the photocatalytic activity of organic photocatalysts, particularly for hydrogen evolution through artificial photosynthesis. It highlights Covalent Organic Frameworks (COFs) as promising materials due to their high surface area, adjustable electronic properties, and stability. The focus is on a regulator-induced amorphous-to-crystalline transformation method to improve the surface crystallization of spherical COFs (SCOFs) for optimal electronic properties. By intensifying the surface crystallinity of COFs through this method, the photocatalytic performance is significantly enhanced, resulting in high hydrogen evolution rates. The study demonstrates that surface crystallinity enhancement prolongs the lifetime of photogenerated charges and reduces electron transfer barriers, ultimately boosting hydrogen evolution efficiency. This surface engineering approach offers a straightforward means of improving the performance of organic photocatalysts without the need for complex molecular design, showcasing a promising avenue for renewable energy applications.