A triboelectric nanogenerator (TENG) can convert energy in the surrounding environment to electricity. Therefore, in recent years, research related to TENGs has significantly increased owing to its simple and low-cost manufacturing process, high portability, and high efficiency. The principle of the TENG lies in the coupling effect of contact electrification and electrostatic induction. Its output performance is directly proportional to the square of the surface charge density, which is related to friction materials. To increase the output power of a TENG and continuously provide electricity for other electronic equipment, many scholars have conducted detailed studies on the triboelectric properties of materials. Particularly, there has been research interest in the chemical functionalization of TENGs due to their unique advantages, such as high triboelectric charge density, durability, stability, and self-cleaning properties. This Progress Report highlights the research progress in chemical modification methods for improving the charge density of TENGs, and classifies their modification methods according to their mechanisms. The effects of chemical reaction, surface chemical treatment, and chemical substance doping on the output performance of TENGs are systematically elaborated. Furthermore, the applications of chemically modified TENG in self-powered sensors and emerging fields, including wearable electronic devices, human-machine interfaces, and implantable electronic devices, are introduced. Lastly, the challenges faced in the future developments of chemical modification methods are discussed, thereby guiding researchers to the use of chemical modification methods for the improvement of charge density for further exploration.