2D van der Waals heterostructures with different types of band alignment have recently attracted great attention due to their unique optical and electrical properties. Most 2D heterostructures are formed by transfer‐stacking two monolayers together, but the interfacial quality and controllable orientation of such artificial structures are inferior to those epitaxial grown heterostructures. Herein, for the first time, a direct vapor phase growth of high‐quality vertically stacked heterostructure of SnS2/MoS2 monolayers is reported. An extremely Type II band alignment exists in this 2D heterostructure, with band offset larger than any other reported. Consistent with the large band offset, distinctive optical properties including strong photoluminescence quenching in the heterostructure area are observed in the heterostructure. The SnS2/MoS2 heterostructures also exhibit well‐aligned lattice orientation between the two layers, forming a periodic Moiré superlattice pattern with high lattice mismatch. Electrical transport and photoresponsive studies demonstrate that the SnS2/MoS2 heterostructures exhibit an obvious photovoltaic effect and possess high on/off ratio (>106), high mobility (27.6 cm2 V−1 s−1) and high photoresponsivity (1.36 A W−1). Efficient synthesis of such vertical heterostructure may open up new realms in 2D functional electronics and optoelectronics.

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The marine internet of things (MIoT), an increasingly important foundation for ocean development and protection, consists of a variety of marine distributed sensors under water. These sensors of the MIoT have always been highly dependent on batteries. To realize in situ power supply, a flexible seaweed-like triboelectric nanogenerator (S-TENG) capable of harvesting wave energy is proposed in this study. The flexible structure, designed with inspiration from the seaweed structure, processes extensive marine application scenarios. The bending and recovering of the S-TENG structure under wave excitations are converted to electricity. As the output performance increases with the number of parallel connected S-TENG units, an S-TENG system with multiple units could serve for floating buoys, coastal power stations, and even submerged devices. Through the demonstration experiments performed in this study, the flexible, low-cost S-TENG could become an effective approach to achieve a battery independent MIoT.