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Two‐dimensional van der Waals heterostructures (2D vdWHs) have recently gained widespread attention because of their abundant and exotic properties, which open up many new possibilities for next‐generation nanoelectronics. However, practical applications remain challenging due to the lack of high‐throughput techniques for fabricating high‐quality vdWHs. Here, we demonstrate a general electrochemical strategy to prepare solution‐processable high‐quality vdWHs, in which electrostatic forces drive the stacking of electrochemically exfoliated individual assemblies with intact structures and clean interfaces into vdWHs with strong interlayer interactions. Thanks to the excellent combination of strong light absorption, interfacial charge transfer, and decent charge transport properties in individual layers, thin‐film photodetectors based on graphene/In2Se3 vdWHs exhibit great promise for near‐infrared (NIR) photodetection, owing to a high responsivity (267 mA W−1), fast rise (72 ms) and decay (426 ms) times under NIR illumination. This approach enables various hybrid systems, including graphene/In2Se3, graphene/MoS2 and graphene/MoSe2 vdWHs, providing a broad avenue for exploring emerging electronic, photonic, and exotic quantum phenomena. [ABSTRACT FROM AUTHOR]