Synchrotron X-ray radiography at 125 frames per second was used to study deformation mechanisms in semi-solid Fe-C alloys at high solid fraction and shear strain rates of 10-1/s. An image correlation approach was also used to quantify the shear strain fields and study shear-induced dilation and the origin of shear cracking. It was shown that, at high solid fraction (90 to 93 pct solid), rearrangement including rotation and translation of solid particles became restricted and shear strain localized into narrow liquid-filled channels/fissures. Shear cracking was shown to originate from inadequate liquid flow into the expanding spaces between solid particles caused by shear-induced dilation. At lower solid fraction (~85 pct solid), solid particles rearranged with a significantly higher component of rotation leading to more shear-induced dilation and a wider shear band.