Harvesting energy from our living environment is an effective approach for sustainable, maintenance-free, and green power source for wireless, portable, or implanted electronics. Mechanical energy scavenging based on triboelectric effect has been proven to be simple, cost-effective, and robust. However, its output is still insufficient for sustainably driving electronic devices/systems. Here, we demonstrated a rationally designed arch-shaped triboelectric nanogenerator (TENG) by utilizing the contact electrification between a polymer thin film and a metal thin foil. The working mechanism of the TENG was studied by finite element simulation. The output voltage, current density, and energy volume density reached 230 V, 15.5 μA/cm 2 , and 128 mW/cm 3 , respectively, and an energy conversion efficiency as high as 10−39% has been demonstrated. The TENG was systematically studied and demonstrated as a sustainable power source that can not only drive instantaneous operation of light-emitting diodes (LEDs) but also charge a lithium ion battery as a regulated power module for powering a wireless sensor system and a commercial cell phone, which is the first demonstration of the nanogenerator for driving personal mobile electronics, opening the chapter of impacting general people's life by nanogenerators. KEYWORDS: Energy harvesting, triboelectric nanogenerator, self-powered system, lithium ion battery A rapid expansion of electronic devices 1−4 toward wireless, portability, and multifunction desperately needs the development of independent and maintenance-free power sources. 5−7 The emerging technologies for mechanical energy harvesting 8−10 are effective and promising approaches for building self-powered systems because of a great abundance of mechanical energy existing in our living environment and human body. Since 2006, piezoelectric nanogenerators (PNGs) 11−14 have been developed to efficiently convert tinyscale mechanical energy into electricity. Recently, another creative invention is the cost-effective and robust triboelectric nanogenerators (TENGs) 15−17 based on the universally known contact electrification effect. 18,19 TENG harvests mechanical energy through a periodic contact and separation of two polymer plates. However, in order to realize sustainable driving of electronic devices/systems, the output of TENG must be significantly improved through a rational design.The two different types of nanogenerators presented above have a similar underlying physical process 12,17 for producing electricity: generation of immobile charges (ionic charges for PNG or electrostatic charges on insulators for TENG), and a periodic separation and contact of the oppositely charged surfaces to change the induced potential across the electrodes, which will drive the flow of free electrons through an external load. The electrical output and efficiency are radically determined by the effectiveness of the above two processes.As for the charge generation in TENG, maximizing the generation of electrostatic charges on opposit...