In this paper, intelligent modeling and analysis of the first principles of high-voltage delithiation of titanium are carried out. The bulk structure of lithium-ion battery cathode materials is simulated and calculated. In order to obtain more accurate lattice constants, we first use the program software package to optimize its structure. Using first principles to delithiate the lithium-ion battery cathode materials the product LixCoO2 and the volume geometry and electronic structure of LixCoO2 have been studied and analyzed in detail. The first principles method based on density functional theory was used to intelligently model the delithiated oxygen vacancies, and the results showed that the accuracy was 96.2%.