The past decade has witnessed remarkable progress in high‐performance Triboelectric nanogenerators (TENG) with the design and synthesis of functional dielectric materials, the exploration of novel dynamic charge transport mechanisms, and the innovative design of architecture, making it one of the most crucial technologies for energy harvesting. High output charge density is fundamental for TENG to expand its application scope and accelerate industrialization; it depends on the dynamic equilibrium of charge generation, trapping, de‐trapping, and migration within its core components. Here, this review classifies and summarizes innovative approaches to enhance the charge density of the charge generation, charge trapping, and charge collection layers. The milestone of high charge density TENG is reviewed based on material selection and innovative mechanisms. The state‐of‐the‐art principles and techniques for generating high charge density and suppressing charge decay are discussed and highlighted in detail, and the distinct charge transport mechanisms, the technologies of advanced materials preparation, and the effective charge excitation strategy are emphatically introduced. Lastly, the bottleneck and future research priorities for boosting the output charge density are summarized. A summary of these cutting‐edge developments intends to provide readers with a deep understanding of the future design of high‐output TENG.