In the present study, to improve the performances of Al0.3CoCrFeNi1.5 high entropy alloys (HEAs), grain boundary character distribution (GBCD) of Al0.3CoCrFeNi1.5 HEA has been optimized by an appropriate thermo-mechanical processing. The experiment results showed that the fraction of low-Σ coincidence site lattice (CSL) boundaries could reach approximately 80 % through cold rolling with deformation of 8 % and subsequent annealing at 1050 °C for 5 min. The reason for GBCD optimization could be attributed to sufficient strain-induced boundary migration (SIBM) or grain growth after recrystallization. While recrystallization is not favorable for optimizing GBCD. The mechanical properties and corrosion resistance have been enhanced, with a more pronounced improvement observed in the corrosion resistance. The corrosion current density icorr of the GBEM specimen stands at 0.23 μA∙cm−2, representing a reduction of 66 % in comparison to the BM specimen (0.68 μA∙cm−2). The improvement of corrosion resistance of Al0.3CoCrFeNi1.5 HEA resulted from the discontinuous random grain boundaries (RGBs) broken by the high fraction of low-ΣCSL boundaries, especially Σ3 boundaries suppressed the propagation of corrosion crack.