Bi‐based nanomaterials have unique physicochemical and structural properties, allowing them to respond to visible light effectively. The Bi‐based semiconductors can be used for degradation of pollutants, reduction of CO2, nitrogen fixation, and decomposition of water, having the strong potential to address environmental pollution and energy shortages. However, the large‐scale application is still limited by the separation and transfer of electron–hole pairs. Herein this review article, carrier dynamics are studied from three perspectives, including structural modulation, atomic conformational reorganization, and surface modification. The relevant mechanisms of different strategies are mainly highlighted, the variations of carrier motion or lifetime are explored, and the progress in practical studies is elucidated. The structural modulation strategy is first introduced, including different dimensional structures and heterogeneous junctions. Further, the atomic conformational reorganization strategy is presented, including Bi‐rich strategies, doping, and vacancy defects. Additionally, the surface modification strategy is outlined, including facet engineering, loading of semiconductor cocatalysts, precious metals, or single atoms. Finally, these strategies are summarized for regulating carrier dynamics and the outlook with the main research trend, providing more inspiration for designing desirable Bi‐based semiconductors.