Aluminum-cobalt co-substituted α-Ni(OH)2 was prepared by means of the titration method in a buffer solution, the structure was characterized by XRD analysis. With above mentioned α-Ni(OH)2 as the positive electrode of a nickel-metal hydride cell, the discharge performances were examined by constant-current charge-discharge experiments. In comparison with the electrodes made of aluminum substituted or cobalt substituted Ni(OH)2 materials, the aluminum-cobalt co-substituted composite electrodes possess an excellent electrochemical performance and are of practical significance.