Abstract Janus structures, named after the ancient two‐faced Roman god Janus, comprise two hemistructures (e.g. hemispheres) with different compositions and functionalities. Much research has been carried out over the past few years on Janus structures because of the intriguing properties and promising potential applications of these unusually shaped materials. This Review discusses recent progress made in the synthesis, properties, and applications of strictly biphasic Janus structures possessing symmetrical structures but made of disparate materials. Depending on the chemical compositions, such biphasic structures can be categorized into soft, hard, and hybrid soft/hard Janus structures of different architectures, including spheres, rodlike, disclike, or any other shape. The main synthetic routes to soft, hard, and hybrid soft/hard Janus structures are summarized and their unique properties and applications are introduced. The perspectives for future research and development are also described.