In the present work, we report for the first time the formation of a dominant Dillamore orientation in a multilayered high-purity aluminum (99.99 %) subjected to an ultra-high von Mises strain of 11.2 by accumulative roll bonding (ARB). This multilayered aluminum with an average layer thickness of 180 nm was produced from an original aluminum sheet thickness of 100 mu m. Microstructure and texture evolutions during ARB processes were investigated in detail and the formation of a dominant orientation is explained. The grain boundary spacing was observed to reduce with increasing number of ARB cycles. However, after 8 ARB cycles, the average grain boundary spacing was measured to be larger than the theoretical layer thickness. Also, a single and strong Cu orientation formed after an intermediate number (8-12) of ARB cycles, which rotated to a dominant Dillamore orientation with further ARB cycles. This is rationalized on the basis of three mechanisms: First, a homogeneous deformation causing lamella structure formation; second, the enhanced dynamic recovery of this pure aluminum through the movement of Y-type triple junction boundaries, resulting in grain coarsening; and third, the coarsening process eliminating the original few and small Brass and S lamellae and simultaneously enhancing the Cu and Dillamore orientations.