Atomic layer deposition (ALD) is an effective method for precise layer‐wise growth of thin‐film materials and has allowed for substantial progress in a variety of fields. Advances in the technique have instigated high‐level interpretations of the relationship between nanostructure architecture and performance. An inherent part in the ALD of films is the underlying interfaces between each material, which plays a significant role in advanced electronics. Considering the impact of sandwiched substructures, it is appropriate to highlight opportunities and challenges faced by applications that rely on these interfaces. This review encompasses the current prospects and obstacles to further performance improvements in ALD‐generated interfaces. 2D electron gas, high‐k materials, freestanding layered structures, lattice matching, and seed layers, as well as prospects for future research, are explored.