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The analysis of structural, electrical transport, critical magnetic behavior, and magnetocaloric properties of Co2CrAl Heusler alloys has been conducted here. Co2CrAl full Heusler alloy has been prepared by the conventional arc melting method in Ar atmosphere and post‐annealing in a vacuum‐sealed quartz tube. X‐ray diffraction (XRD) pattern reveals the crystallization of the alloy to the Fmm space...