Vibrations induced by human motions and vehicle operations feature low-frequency, broadband, and time-varying. However, enhancing the power density of energy harvesting for various low-frequency applications presents a significant challenge. This paper proposes a high-performance dual-mode energy harvester (DM-EH) incorporating coupled nonlinear pendulum and speed-amplified mechanisms with gears for the simultaneous scavenging vibration and rotation energy. The pendulum serves as the energy capture unit for detecting vibration energy while ensuring the effective operation of the generation unit in rotational environments. The gears amplify the speed of the excitation and enable frequency up-conversion, thereby enhancing the energy conversion. Experimental results substantiate the DM-EH's ability to extract power from vehicle operations at speeds ranging from 60 to 540 rpm, as well as from human motions at frequencies of 0.7 to 1.5 Hz with 30° amplitudes. In rotation mode, the prototype achieves a maximum average direct current power of 3.79 W, while in vibration mode, it attains 244 mW. The prototype successfully powers portable electronics and supports battery-free triaxial acceleration and temperature multi-sensors during human motions and railway simulation tests. This prototype showcases immense potential as a sustainable power source for portable electronics and self-powered monitoring applications.