Nature has evolved hierarchical structures of hybrid materials with excellent mechanical properties. Inspired by nacre’s architecture, a ternary nanostructured composite has been developed, wherein stacked lamellas of 1D vanadium pentoxide nanofibres, intercalated with water molecules, are complemented by 2D graphene oxide (GO) nanosheets. The components self-assemble at low temperature into hierarchically arranged, highly flexible ceramic-based papers. The papers’ mechanical properties are found to be strongly influenced by the amount of the integrated GO phase. Nanoindentation tests reveal an out-of-plane decrease in Young’s modulus with increasing GO content. Furthermore, nanotensile tests reveal that the ceramic-based papers with 0.5 wt% GO show superior in-plane mechanical performance, compared to papers with higher GO contents as well as to pristine V2O5 and GO papers. Remarkably, the performance is preserved even after stretching the composite material for 100 nanotensile test cycles. The good mechanical stability and unique combination of stiffness and flexibility enable this material to memorize its micro- and macroscopic shape after repeated mechanical deformations. These findings provide useful guidelines for the development of bioinspired, multifunctional systems whose hierarchical structure imparts tailored mechanical properties and cycling stability, which is essential for applications such as actuators or flexible electrodes for advanced energy storage.