In this article, the structural and chemical properties of heterogeneous catalysts prepared by atomic layer deposition (ALD) are discussed. Oxide shells can be deposited on metal particles, forming shell/core type catalysts, while metal nanoparticles are incorporated into the deep inner parts of mesoporous supporting materials using ALD. Both structures were used as catalysts for the dry reforming of methane (DRM) reaction, which converts CO2 and CH4 into CO and H2. These ALD-prepared catalysts are not only highly initially active for the DRM reaction but are also stable for long-term operation. The origins of the high catalytic activity and stability of the ALD-prepared catalysts are thoroughly discussed.