In many nano(opto)electronic devices, the roughness at surfaces and interfaces is of increasing importance, with roughness often contributing toward losses and defects, which can lead to device failure. Consequently, approaches that either limit roughness or smoothen surfaces are required to minimize surface roughness during fabrication. The atomic-scale processing techniques atomic layer deposition (ALD) and atomic layer etching (ALE) have experimentally been shown to smoothen surfaces, with the added benefit of offering uniform and conformal processing and precise thickness control. However, the mechanisms which drive smoothing during ALD and ALE have not been investigated in detail. In this work, smoothing of surfaces by ALD and ALE is studied using finite difference simulations that describe deposition/etching as a front propagating uniformly and perpendicular to the surface at every point. This uniform front propagation model was validated by performing ALD of amorphous Al 2 O 3 using the TMA/O 2 plasma. ALE from the TMA/SF 6 plasma was also studied and resulted in faster smoothing than predicted by purely considering uniform front propagation. Correspondingly, it was found that for such an ALE process, a second mechanism contributes to the smoothing, hypothesized to be related to curvature-dependent surface fluorination. Individually, the atomic-scale processing techniques enable smoothing; however, ALD and ALE will need to be combined to achieve thin and smooth films, as is demonstrated and discussed in this work for multiple applications.