The implementation of control over self‐separation of thick GaN flayers grown by Hydride Vapor‐Phase Epitaxy (HVPE) on Metal‐Organic Chemical Vapor Deposition (MOCVD)‐grown templates with patterned nano‐column interlayer is reported. Both numerical simulation and experimental data show that separation of thick HVPE layers is provided by non‐uniform redistribution of the growth stress. It is shown that the geometrical parameters of the nano‐column structure such as fill factor and shape of the columns are most critical for self‐separation effect. By adjusting the nano‐column pattern, successful self‐separation of thick HVPE layers from 2‐inch structured MOCVD GaN/sapphire substrate was demonstrated. (© 2014 WILEY‐VCH Verlag GmbH & Co. KGaA, Weinheim)