The low toughness and structural stability of nanostructured materials is strongly related to the numerous grain boundaries and interfaces. This necessitates new design strategies to inherently improve the grain boundaries. Amongst other concepts the use of low‐energy boundaries has turned out to provide the most comprehensive improvement of the property spectrum targeting on ductility, toughness, as well as thermal and microstructural stability upon mechanical loading. Cyclic high‐pressure torsion (CHPT) is one prosperous technique to synthesis low‐angle boundaries (LAGB) at the nanoscale, enabling the production of high‐strength materials. We present here an in‐depth analysis of the structural evolution focusing on the effect of different strain amplitudes and accumulated strains as well as crystal structure to understand how these parameters need to be adjusted to optimize the fraction of LAGBs. Different than expected from classical fatigue testing, the crystal structure seems to play a minor role for the cell structure evolution at comparably large strain amplitudes. It is therefore a strong asset that CHPT is feasible to produce nanostructures LAGB boundaries in both FCC and BCC structures. Furthermore, by optimizing the geometry of the anvils, it enables homogenous structural sizes in the entire sample as in contrast to other techniques the strain gradient impact on LAGB formation can be overcome.This article is protected by copyright. All rights reserved.