Enhanced workability, as characterized by the magnitude and heterogeneity of accommodated plastic strains during sheet processing, is demonstrated in high Si content Fe-Si alloys containing 4 and 6.5 wt% Si using two single-step, simple-shear deformation techniques – peeling and large strain extrusion machining (LSEM). The model Fe-Si material system was selected for its intrinsically poor material workability, and well-known applications potential in next-generation electric machines. In a comparative study of the deformation characteristics of the shear processes with conventional rolling, two distinct manifestations of workability are observed. For rolling, the relatively diffuse and unconfined deformation zone geometry leads to cracking at low strains, with sheet structures characterized by extensive deformation twinning and banding. Workpiece pre-heating is required to improve the workability in rolling. In contrast, peeling and LSEM produce continuous sheet at large plastic strains without cracking, the result of more confined deformation geometries that enhances the workability. Peeling, however, results in heterogeneous, shear-banded microstructures, pointing to a second type of workability issue – flow localization – that limits sheet processing. This shear banding is to a large extent facilitated by unrestricted flow at the sheet surface, unavoidable in peeling. With additional confinement of this free surface deformation and appropriately designed deformation zone geometry, LSEM is shown to suppress shear banding, resulting in continuous sheet with homogeneous microstructure. Thus LSEM is shown to produce the greatest enhancement in process workability for producing sheet. These workability findings are explained and discussed based on differences in process mechanics and deformation zone geometry.