development. As two important renewable energy sources, wind energy and solar energy have achieved unprecedented development in the past decade. However, the large-scale construction of wind and solar power station will occupy the limited land resources, and have a certain impact ecological environment. As the main form in the earth's surface, ocean contains enormous pollution-free and renewable blue energy such as wave energy, [2] which have many advantages, such as large reserves, reliable predictability, and wide distribution. More importantly, large-scale marine power station construction will not only occupy our limited land resources, and can reduce the erosion of wave on the coast, meanwhile it can provide sufficient power in situ for the development of marine resources and marine monitoring. The linear permanent magnet generators, which is widely studied technology for harvesting wave energy, generally suffers from high cost, complex installation process, and poor energy harvest efficiency in low frequency. [3] Based on the advantages of lightweight , [4] low cost, [5,6] simple structure, [7] diverse material options [8] and high efficiency at the low-frequency, [3] the triboelectric nanogenerator (TENG) is widely applied in the micro/nanoenergy, [5,6] selfpowered sensing, [9] environmental protection, and flexible electronics applications. [10] Meanwhile, with the merits of lightweight, [4] low-cost, [5,6] and high-efficiency in low frequency (<5 Hz), [3] TENG, based on the triboelectrification effect and electrostatic induction, [11-13] shows many superiorities in wave energy harvesting. [14,15] Therefore, TENG (Figure S1A, Supporting Information) has been regarded as a potential technology instead of linear permanent magnet generators for harvesting low-frequency water wave energy. [16-20] As an energy harvester, the commercialization application of TENG highly depends on their volume power density, which is proportionally related to the space utilization and the triboelectric charge density. Hence, many works have been done to improve the volume power density of TENG. Spring structures (Figure S1B, Supporting Information) were designed for generating a highfrequency output, [21-24] but they suffer from large damping coefficient. A 3D electrode structure [25] was used to enhance the space utilization, and soft silica ball [26] and multilayered structure [22] were applied for increasing the effective triboelectric surface area. Based on these structures of optimization, the Triboelectric nanogenerators (TENGs) have been introduced as a new costeffective technology for harvesting renewable wave energy for their unmatchable performance in low frequency (<5 Hz). Here, bifilar-pendulum-assisted multilayer-structured triboelectric nanogenerator (BM-TENG) modules incorporated into a vessel for wave energy harvesting are reported, which have a high output performance and adaptive capacity in actual marine environment. Compared with previous research work on wave energy collection by TENG, the designed BM-TENG,...