The energy dissipated by virialisation shocks during hierarchical structure formation of the Galaxy can exceed that injected by concomitant supernova (SN) explosions. Cosmic rays (CRs) accelerated by such shocks may therefore dominate over SNe in the production of 6Li through α + α fusion without co-producing Be and B. This process can give a more natural account of the observed 6Li abundance in metal-poor stars compared to standard SN CR scenarios. Future searches for correlations between the 6Li abundance and the kinematic properties of halo stars may constitute an important probe of how the Galaxy and its halo formed. Furthermore, 6Li may offer interesting clues to some fundamental but currently unresolved issues in cosmology and structure formation on sub-galactic scales.