Plasma-based atomic layer etching of materials may be of benefit to various semiconductor manufacturing and related technologies. For example, plasma-based atomic layer etching of materials may be beneficial for adding and/or removing angstrom thick layers from a surface in advanced semiconductor manufacturing and related technologies that increasingly demand atomistic surface engineering. A method may include depositing a controlled amount of a chemical precursor on an unmodified surface layer of a substrate to create a chemical precursor layer and a modified surface layer. The method may also include selectively removing a portion of the chemical precursor layer, a portion of the modified surface layer and a controlled portion of the substrate. Further, the controlled portion may be removed to a depth ranging from about 1/10 of an angstrom to about 1 nm. Additionally, the deposition and selective removal may be performed under a plasma environment.