Triboelectric nanogenerator (TENG) has received tremendous attention in ambient energy harvesting, especially for ocean wave energy. However, the technology is generally challenged to obtain excellent durability and high efficiency simultaneously, which primarily overshadows their further industrial‐scale applications. Here, a dual‐mode and frequency multiplied TENG with ultrahigh durability and efficiency for ultralow frequency mechanical energy harvesting via the elastic connection and soft contact design is proposed. By introducing the spring and flexible dielectric fluff to the novel pendulum‐like structural design, the surface triboelectric charges of TENG are replenished in soft contact mode under the intermittent mechanical excitation, while the robustness and durability are enhanced in non‐contact working mode. The fabricated TENG results in a continuous electrical output for 65 s by one stimulus with a high energy conversion efficiency, as well as negligible change of output performance after a total of 2 000 000 cycles. Moreover, integrated with the power management circuit, the TENG array is demonstrated to drive the electronics by effectively harvesting wind and water wave energy as a sustainable energy source. This work paves a new pathway to enhance the robustness, durability, and efficiency of the TENG that resolves the bottleneck of its practical applications and industrialization.

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