In situ nano-TiB2 reinforced ultrafine-grained (UFG) Al composites were prepared via combined processes of flux-assisted synthesis (FAS) and asymmetrical rolling (ASR). The UFG Al composite with an ASR reduction ratio of 97% exhibits an average matrix grain size of 380 nm and an average TiB2 particulate size of 50 nm. Dislocation density in the composites is higher than that corresponding to the high purity (99.99 wt%) Al under identical processing conditions. The yield and ultimate tensile strength values of the UFG Al composites processed with an ASR reduction ratio of 97% are approximately 9 and 5 times higher relative to those of the initial coarse-grained Al, respectively. Moreover, the UFG Al composite with an ASR reduction ratio of 97% exhibits a higher elongation than that corresponding to the UFG pure Al under identical processing conditions, suggesting that nanoparticulates contribute to the overall plastic deformation when the matrix grains are refined to the UFG regime. Moreover, analysis of the strengthening behavior reveals no clear evidence that Orowan strengthening contributes significantly to the overall yield strength of the Al nanocomposites studied herein.