Recently, silver nanoparticles (AgNPs) have been widely applied in sterilization due to their excellent antibacterial properties. However, AgNPs require rigorous storage conditions because their antibacterial performances are significantly affected by environmental conditions. Instant fabrication provides a remedy for this drawback. In this study, we propose a self-powered electrodeposition system to synthesize sub-10-nm AgNPs, consisting of a triboelectric nanogenerator (TENG) as the self-powered source, a capacitor for storing electrical energy from the TENG, and an electrochemical component for electrodeposition. The self-powered system with larger capacitance and discharging voltage tends to deliver smaller AgNPs due to the nucleation mechanism dominated by current density. Furthermore, antibacterial tests reveal that compared to direct current (DC) electrodeposition, the TENG-based electrodeposition can synthesize finer-sized AgNPs (<10 nm) with overwhelming antibacterial effect against Escherichia coli (E. coli) and Staphylococcus aureus (S. aureus) (with 100% efficiency at 2 h). This work provides a new strategy for the self-powered, instant, and controllable electrodeposition of nanoparticles.