In this paper, crack‐free GaN films with step‐graded AlGaN transition layer and AlGaN superlattice layer as buffer layers were grown on Si(111) substrate by metal‐organic chemical vapor deposition(MOCVD). The combination of both buffers effectively improves the properties of GaN layer. With the optimization of the buffer structures, high quality compressively‐strained GaN layers with thickness up to 3.6 μm have been obtained on Si(111) substrates (© 2015 WILEY‐VCH Verlag GmbH & Co. KGaA, Weinheim)