Refinement of grain size is one of the biggest challenges to produce steels with improved combination of strength and toughness. Ultrafine structures are being produced world-wide on various materials, including low carbon steel, using different types of processes. However, the majority of these processes also exhibit severe limitations because they are generally restricted to small samples and are difficult to be implemented on an industrial scale. A promising technique for industrial implementation is the Accumulative Roll Bonding (ARB), a process able to supply large samples, even in the laboratory scale. In this paper, warm intense straining (ε = 4) by ARB was applied to a plain low-C steel in order to develop ultrafine grains, aiming at sizes around 1-2 μm, suitable to maintain an adequate combination of strength and ductility. The effect of annealing conditions on the evolution of the work-hardened microstructure and the bonding behaviour after each pass were investigated. Orientation Imaging Microscopy was used to investigate the microstructure and give a quantitative assessment of high angle and low angle boundaries. It is showed that the frequency of high angle grain boundaries increases with the strain but the misorientation distribution remained far from that typical of a recrystallised material.