We demonstrated a hybrid nanogenerator (NG) exploiting both piezoelectric and triboelectric effects induced from ZnO nanoflakes (NFs)/polydimethylsiloxane (PDMS) composite films through a facile, cost-effective fabrication method. This hybrid NG exhibited not only high piezoelectric output current owing to the enhanced surface piezoelectricity of the ZnO NFs but also high triboelectric output voltage owing to the pronounced triboelectrification of Au–PDMS contact, producing a peak-to-peak output voltage of ∼470 V, a current density of ∼60 μA·cm–2, and an average power density of ∼28.2 mW·cm–2. Without additional energy storage devices, the hybrid NGs with an area of 3 × 3 cm2 instantaneously lit up 180 commercial green light-emitting diodes through periodic hand compression. This approach may provide an innovative design for constructing high-performance and portable energy harvesting devices with enhanced power output, scavenging ambient mechanical energy from human motions in our daily life.