Recently, novel high‐entropy alloys (HEAs) of Al–Co–Cr–Fe–Ni–Ti systems containing face‐centered cubic (FCC) matrix and γ′ precipitates (L1 2 phase) have been studied. They show superior mechanical properties at room (298 K) and cryogenic temperatures (77 K). Herein, microstructure deformation and fracture after tensile strain are investigated. The results show that multiple‐layered stacking faults occur after the tensile test at 77 K, which can increase the yield strength and ultimate tensile strength by 20% and 24%, respectively. The γ′ precipitates become disordered after the alloy deforms at 77 K, which decreases the formation barrier of mechanical twinning and increases ductility at 77 K by 27%.