. IntroductionOver the past decades, harvesting ambient environmental energy has attracted increasing interest for realizing self-powered systems and for meeting large-scale energy demands. Searching for clean and renewable energy with reduced carbon emissions is urgent to the sustainable development of human civilization. [ 1 ] To date, various energy harvesters for scavenging ambient environmental vibrational energy have been developed that rely on piezoelectric, [2][3][4][5][6] electromagnetic, [ 7,8 ] and electrostatic [ 9,10 ] transduction mechanisms. Considerable research effort has been devoted to improve the effi ciency of vibrational energy harvesters. [11][12][13][14][15][16][17][18] However, regardless of the transduction mechanisms and novel structures, the vibration-to-electric conversion effi ciency is still quite low in the existing harvesters because: 1) most of them are designed as linear resonant structures in order to achieve maximum power generation, which limits their application in realworld environments with stochastic or varying vibration spectra; [ 14 ] and 2) most devices can only effectively harvest vibrational energy from a single motion direction and/or within a small bandwidth. In this case, the harvesters are not effective at scavenging energy from a vibration with multiple or time-variant motion directions. [ 11,12,14 ] Recently, the innovative triboelectric nanogenerator (TENG) has offered a costeffective, simple, and robust approach to convert mechanical energy into electricity based on the coupling between triboelectrifi cation and electrostatic induction. [19][20][21][22][23][24][25][26][27] The triboelectrically charged planes of TENGs change the electric polarization and fi eld across two electrodes by either periodic vertical contact separation [19][20][21] or in-plane sliding, [ 22,23 ] leading to an alternating fl ow of electrons through the external load. The developed TENGs have been successfully applied as sustainable power sources for portable electronics, [ 21 ] magnetic sensors, [ 24 ] environmental monitors, [ 25 ] and other self-powered systems. [ 26,27 ] Here, we demonstrated a newly designed 3D-TENG that is able to scavenge vibrational energy in the out-of-plane direction and arbitrary in-plane directions with considerable wide bandwidth. It works in a hybridized mode of both vertical contact separation and in-plane sliding. Under out-of-plane motion excitation, the 3D-TENG produces an open-circuit voltage up to 123 V, a peak short-circuit current density of 30 mA m −2 , and a peak power density of 1.35 W m −2 . The corresponding electrical outputs are 143 V, 32 mA m −2 , and 1.45 W m −2 , respectively, when the 3D-TENG works under in-plane motion excitation. The remarkable performance enables the 3D-TENG to have tremendous practical applications including harvesting windor rain-droplet-induced vibrational energy from the national grid transmission lines, natural vibration energy from human walking, and rotation energy from vehicles with wheels.