Energy harvesting and storage are the two most important energy technologies developed for portable, sustainable, and self-sufficient power sources for mobile electronic systems. However, both have limitations for providing stable direct-current (DC) with an infinite lifetime. Herein, we integrated a triboelectric nanogenerator (TENG)-based mechanical energy harvester with Li-ion-battery (LIB)-based energy storage as a single device for demonstrating a flexible self-charging power unit (SCPU), which allows a battery to be charged directly by ambient mechanical motion. This physical integration enables a new operation mode of the SCPU: the “sustainable mode”, in which the LIB stores the TENG-generated electricity while it is driving an external load. With the LIB being replenished by the ambient mechanical energy, the SCPU can keep providing a constant voltage to the load by utilizing the stable difference between the battery’s intrinsic electrode potentials. This study will impact the traditional trends of battery research and advance the development of the self-powered systems.