In response to the growing demand for high-performance lithium-ion batteries, this study investigates the crucial role of different carbon sources in enhancing the electrochemical performance of lithium iron phosphate (LiFePO4) cathode materials. Lithium iron phosphate (LiFePO4) suffers from drawbacks, such as low electronic conductivity and low lithium-ion diffusion coefficient, which hinder its industrial development. Carbon is a common surface coating material for LiFePO4, and the source, coating method, coating amount, and incorporation method of carbon have a significant impact on the performance of LiFePO4 materials. In this work, iron phosphate was used as the iron and phosphorus source, and lithium carbonate was used as the lithium source. Glucose, phenolic resin, ascorbic acid, and starch were employed as carbon sources. Ethanol was utilized as a dispersing agent, and ball milling was employed to obtain the LiFePO4 precursor. Carbon-coated LiFePO4 cathode materials were synthesized using the carbothermal reduction method, and the effects of different carbon sources on the structure and electrochemical performance of LiFePO4 materials were systematically investigated. The results showed that, compared to other carbon sources, LiFePO4 prepared with glucose as the carbon source not only had a higher discharge specific capacity but also better rate cycle performance. Within a voltage range of 2.5–4.2 V, the initial discharge specific capacities at 0.1, 0.5, and 1 C rates were 154.6, 145.6, and 137.6 mAh/g, respectively. After 20 cycles at a 1 C rate, the capacity retention rate was 98.7%, demonstrating excellent electrochemical performance.