Janus structures that include different functional compartments have attracted significant attention due to their specific properties in a diverse range of applications. However, it remains challenge to develop an effective strategy for achieving strong interfacial interaction. Herein, a Janus nanoreactor consisting of TiO2 2D nanocrystals integrated with Prussian blue analog (PBA) single crystals is proposed and synthesized by mimicking the planting process. In situ etching of PBA particles induces nucleation and growth of TiO2 nanoflakes onto the concave surface of PBA particles, and thus enhances the interlayer interaction. The anisotropic PBA–TiO2 Janus nanoreactor demonstrates enhanced photocatalytic activities for both water reduction and oxidation reactions compared with TiO2 and PBA alone. As far as it is known, this is the first PBA‐based composite that serves as a bifunctional photocatalyst for solar water splitting. The interfacial structure between two materials is vital for charge separation and transfer based on the spectroscopic studies. These results shed light on the elaborate construction of Janus nanoreactor, highlighting the important role of interfacial design at the microscale level.
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