Extrusion machining (EM) is an efficient and convenient method to prepare ultrafine-grained (UFG) materials. As a vital parameter in the EM process, tool rake angle (α) is critical to control the material's shear strain and grain size. The grains tend to refine with decreasing α, whereas a small α leads to difficult cutting, chip breakage, and poor surface quality. To achieve the controllable strain distribution, grain size adjustment, and improved formability of UFG pure copper strips, this paper proposed a novel design of the variable rake angle (VRA) tool. Combining experiments and finite element simulation, extrusion machining with variable rake angle tools (VRA-EM) was investigated. The results implied that a deviating angle (β) for the material flow existed during VRA-EM. The β increased as the cutting thickness (tc) increased, resulting in decreased plastic deformation, strain, and microhardness. The microstructure was also characterized by electron backscatter diffraction system (EBSD) and transmission electron microscopy (TEM) techniques. A dead metal zone was formed using the VRA tool, in which the material flow behavior was quite weak. The obtained UFG strip was further divided into the low-strain zone (LSZ) and high-strain zone (HSZ) based on strain distribution. And a new theoretical model of shear strain was established and conformed to experimental values. Accordingly, VRA-EM process was able to improve the mechanical properties and strain controllability, showing promising prospects for efficiently fabricating UFG materials.