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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 group with L2₁ crystal symmetry. The correspondence between the magnetic and electrical transport properties of the Co₂CrAl alloy has been observed. This alloy exhibits paramagnetic to ferromagnetic transition (Curie temperature) just above room temperature at around 340 K. Metallic to semiconducting transition occurs near the magnetic Curie temperature. Critical magnetic behavior has been analyzed by employing the Arrott plot, Kouvel–Fisher methods, and critical isotherm analysis. These conclude that the …