Laser-driven ion sources are approaching the requirements for several applications in materials and nuclear science. Relying on compact, table-top, femtosecond laser systems is pivotal to enable most of these applications. However, the moderate intensity of these systems (I10 19 W cm −2 ) could lead to insufficient energy and total charge of the accelerated ions. The use of solid foils coated with a nanostructured near-critical layer is emerging as a promising targeted solution to enhance the energy and the total charge of the accelerated ions. For an appropriate theoretical understanding of this acceleration scheme, a realistic description of the nanostructure is essential, also to precisely assess its role in the physical processes at play. Here, by means of 3D particle-in-cell simulations, we investigate ion acceleration in this scenario, assessing the role of different realistic nanostructure morphologies, such as fractal-like foams and nanowire forests. With respect to a simple flat foil, the presence of a nanostructure allows for up to a×3 increase of the maximum ion energy and for a significant increase of the conversion efficiency of laser energy into ion kinetic energy. Simulations show also that the details of the nanostructure morphology affect both the maximum energy of the ions and their angular distribution. Furthermore, combined 3D particle-in-cell and Monte Carlo simulations show that if accelerated ions are used for neutron generation with a beryllium converter, double-layer nanostructured targets allow to greatly enhance the neutron yield. These results suggest that nanostructured double-layer targets could be an essential component to enable applications of hadron sources driven by compact, table-top lasers. feasibility of laser-driven ion beam analysis for non-destructive materials characterization. Laser-driven ion sources have been considered to test electronic components in a harsh radiation environment [18], for thermal stress testing [19], to study ultra-fast dynamics in irradiated materials [20,21], and for materials synthesis [22,23]. Ultrashort pulsed neutron sources driven by laser-accelerated ions [24-32] have been investigated for applications such as fast neutron spectroscopy [33] and radiography [34].What make these applications particularly attractive are the requirements for the ion source. Energies of few MeVs are perfectly suitable for several ion beam analysis techniques [35] or to generate neutrons with a lithium [36] or beryllium [37] converter. Moreover, for selected applications, the inherently broad energy spectrum of a laser-driven ion source [2] is not detrimental [15,17] and could even be beneficial [18]. Maximum ion energies of ∼1 MeV have been recently demonstrated even with commercial, sub-terawatt laser systems [38]. These lasersystems are truly table-top and can operate at a high repetition rate (kiloHertz). Relying on these systems could make laser-driven ion sources portable and competitive with conventional accelerators, paving the way for their widesprea...