In this work, the effect of the Al content (x = 5, 10, and 15 at. %) on the martensitic transformation (MT) and microstructure and mechanical properties of Cu(50−x)Zr50Alx alloys was studied. The microstructure of the alloys was characterized at room temperature by means of scanning electron microscopy and X-ray diffraction. An increase in Al content reduces the amount of transforming CuZr phase, and consequently the secondary phase formation is favored. The evolution of the MT upon thermal cycling was investigated as a function of the Al content by differential scanning calorimetry. MT temperatures and enthalpies were found to be decreased when increasing the Al content. Al addition can induce a sudden, stable MT below 0 °C, while the binary alloy requires ten complete thermal cycles to stabilize. Finally, the mechanical properties were investigated through microhardness and compression testing. No linear dependence was found with composition. Hardness lowering effect was observed for 5–10 at. % of Al content, while the hardness was increased only for 15 at. % Al addition with respect to the binary alloy. Similarly, compressive response of the alloys showed behavior dependent on the Al content. Up to 10 at. % Al addition, the alloys indicate a superelastic response at room temperature, while higher Al content induced untimely failure.