Wave motion in the ocean can generate plentiful energy, but it is difficult to harvest wave energy for practical use because of the low frequency and random directional characteristics of wave motion. In this paper, a gyroscope-structured triboelectric nanogenerator (GS-TENG) is proposed for harvesting multidirectional ocean wave energy. Its inner and outer generation units can operate independently in different directions, and they all adopt the friction mode of surface contact. While realizing noninterference multidirectional energy harvesting, the power generation area is increased. In the experiments, under acceleration of 6 m/s2 with variations in excitation angle, the GS-TENG can output direct currents of 0.8–3.2 μA, and the open-circuit voltages of the inner and outer generation units can reach 730 and 160 V, respectively. When the devices are networked and placed in the water, the electrical energy generated by the GS-TENGs can enable commercial thermometers to operate normally. The attenuation of direct-current output by the GS-TENG in the experiment of 30 days in water is about 8%, which verifies the good durability of the device in the water environment. Therefore, the GS-TENG has excellent application prospects in the wave energy harvesting field.