The presence of open-volume defects, such as vacancies, can significantly alter the functional properties of a material, including its structure and electronic transport. This study employs ion irradiation using inert ions (Ar⁺) and transition metal ions (Co⁺) at fluences of 10¹²-10¹⁵ions· cm^-2 to achieve systematic disorder in the multilayer structure of MAX-phase Cr₂AlC. It is shown that the magnitude of the paramagnetic response of Cr₂AlC increases with ion fluence, regardless of the dopant used. A combination of isolated moments in defect sites with J=1/2 and magnetic clusters are used to explain this behavior. Low-temperature (< 30 K) resistivity measurements show local minima and sudden up(down)-turns with decreasing temperature, which, together with unusual MR in this temperature range, suggest the presence of quantum transport effects, such as the Kondo effect.