We have performed first-principles calculations of the atomic and electronic structures and stability of three (alpha, beta and gamma) layered V2O5 phases and their free layers within the same computational approach. In computations, we have used a hybrid exchange correlation functional within the density functional theory and a basis set of localized atomic orbitals. All the lattice parameters and the atomic positions have been totally optimized and the phonon frequencies at the Gamma-point of the Brillouin zone have been obtained. The calculated relative stability of considered bulk phases decreases as alpha > gamma > beta. The calculated relative stability of layers differs from that of bulk phases and decreases as beta > alpha >= gamma. The possibility of the folding of V2O5 layers into nanotubes is discussed. (C) 2014 Acta Materialia Inc. Published by Elsevier Ltd. All rights reserved.