Low-angle grain boundaries (LAGBs) accommodate residual stress through the rearrangement and accumulation of dislocations during cold rolling. This study presents an electron wind force-based annealing approach to recover cold-rolling induced residual stress in FeCrAl alloy below 100 °C in 1 min. This is significantly lower than conventional thermal annealing, which typically requires temperatures around 750 °C for about 1.5 h. A key feature of our approach is the athermal electron wind force effect, which promotes dislocation movement and stress relief at significantly lower temperatures. The electron backscattered diffraction (EBSD) analysis reveals that the concentration of low-angle grain boundaries (LAGBs) is reduced from 82.4% in the cold-rolled state to a mere 47.5% following electropulsing. This level of defect recovery even surpasses the pristine material’s initial state, which exhibited 54.8% LAGBs. This reduction in LAGB concentration was complemented by kernel average misorientation (KAM) maps and X-ray diffraction (XRD) Full Width at Half Maximum (FWHM) measurements, which further validated the microstructural enhancements. Nanoindentation tests revealed a slight increase in hardness despite the reduction in dislocation density, suggesting a balance between grain boundary refinement and dislocation dynamics. This proposed low-temperature technique, driven by athermal electron wind forces, presents a promising avenue for residual stress mitigation while minimizing undesirable thermal effects, paving the way for advancements in various material processing applications.