The activation of the C−H bond, a necessary step to get high-value-added compounds, is one of the most important issues in modern catalysis. Combining the advantages of both homogeneous and heterogeneous catalysis, a certain continuous homogeneous process should be one of the ideal routes for the catalytic activation of C−H bonds. Here, through machine learning (ML), we predicted and fabricated metal-free carbon dot (C-Dot) homogeneous catalysts for C−H bond oxidation. These C-Dots have an ascorbic acid unit based polymer-like structure with a polymerization degree in the range of 3−10. With C-Dots as the catalyst, three groups (aliphatic, aromatic, and cycloalkanes) of 10 hydrocarbon molecules were tested, proving its generality for the catalytic oxidation of the C−H bond. A typical example of cyclohexane that was selectively oxidized to adipic acid (AA) by using a circulation and phase-transfer process demonstrates its critical advantages, such as the continuous and large-scaled producing ability of the homogeneous catalysis process. The one-pass conversion efficiency of cyclohexane to AA reaches 77.49% with selectivity up to 84.24% in 4 h. The yield of 16.32% per hour is about 4 times over that of modern technology. Theoretical calculations suggested that the O 2 activation on C-Dots plays a crucial role in determining the reaction rate of the entire catalytic oxidation process of cyclohexane.