Samples of pure aluminium (99.99%) have been produced by accumulative roll-bonding to a large strain followed by a heat treatment, where a two-step annealing process has been used to produce samples with large variations in structural parameters such as boundary spacing, misorientation angle and dislocation density. These parameters have been quantified by a structural analysis applying transmission electron microscopy and electron backscatter diffraction, and the mechanical properties have been determined by tensile testing at room temperature. Strength-structure relationships have been analysed based on the operation of two strengthening mechanisms-grain boundary and dislocation strengthening-and good agreement with experiments has been found for the deformed sample. However, for samples where the density of dislocation sources has been reduced significantly by annealing, an additional strengthening mechanism, so-called dislocation source-limited hardening, may operate as a higher stress is required to activate alternative dislocation sources. © 2009 Acta Materialia Inc.