The tailoring of the metal–oxide interface is an important strategy in the design and development of novel catalysts with superior catalytic performance. However, the structure and location of the metal–oxide interface on supported catalysts cannot be well controlled by traditional methods, and the structure–property relation is not clearly understood in most reactions. Therefore, it is highly desirable to develop new methods to precisely tailor the metal–oxide interface and thus achieve highly efficient catalysts and a fundamental understanding of the principle of interface catalysis. Atomic layer deposition (ALD), a high-level film-growth technology, is a promising and controllable approach to precisely design and tailor the metal–oxide interface on an atomic scale. In this Review, we present and discuss a series of recently developed ALD strategies for tailoring the metal–oxide interface of heterogeneous catalysts, such as overcoating, ultrathin modification, area-selective ALD, template-assisted ALD, and template- and sacrificial-layer-assisted ALD. These methods have been used to develop many catalysts with different structures, such as core–shell structures, inverse oxide/metal structures, oxide–nanotrapped metal structures, porous sandwich structures, multiply confined metal nanoparticles in oxide nanotubes, and multifunctional catalysts with multiple metal–oxide interfaces. Due to its advantages, ALD can be applied to reveal the catalytic mechanism of metal–oxide interfaces by deliberately designing catalysts with a clear structure, even in confined and synergetic environments. In general, the developed ALD approaches provide us with a toolkit for tailoring the metal–oxide interface and designing heterogeneous catalysts.