AbstractTo sustainably power electronics by harvesting mechanical energy using nanogenerators, energy storage is essential to supply a regulated and stable electric output, which is traditionally realized by a direct connection between the two components through a rectifier. However, this may lead to low energy-storage efficiency. Here, we rationally design a charging cycle to maximize energy-storage efficiency by modulating the charge flow in the system, which is demonstrated on a triboelectric nanogenerator by adding a motion-triggered switch. Both theoretical and experimental comparisons show that the designed charging cycle can enhance the charging rate, improve the maximum energy-storage efficiency by up to 50% and promote the saturation voltage by at least a factor of two. This represents a progress to effectively store the energy harvested by nanogenerators with the aim to utilize ambient mechanical energy to drive portable/wearable/implantable electronics.