Atomic layer deposition (ALD) is a deposition technique well‐suited to produce high‐quality thin film materials at the nanoscale for applications in transistors. This review comprehensively describes the latest developments in ALD of metal oxides (MOs) and chalcogenides with tunable bandgaps, compositions, and nanostructures for the fabrication of high‐performance field‐effect transistors. By ALD various n‐type and p‐type MOs, including binary and multinary semiconductors, can be deposited and applied as channel materials, transparent electrodes, or electrode interlayers for improving charge‐transport and switching properties of transistors. On the other hand, MO insulators by ALD are applied as dielectrics or protecting/encapsulating layers for enhancing device performance and stability. Metal chalcogenide semiconductors and their heterostructures made by ALD have shown great promise as novel building blocks to fabricate single channel or heterojunction materials in transistors. By correlating the device performance to the structural and chemical properties of the ALD materials, clear structure–property relations can be proposed, which can help to design better‐performing transistors. Finally, a brief concluding remark on these ALD materials and devices is presented, with insights into upcoming opportunities and challenges for future electronics and integrated applications.