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This invention provides a composite electrode for the comprehensive recovery of valuable metals, its preparation method, and its application. The composite electrode comprises a positive electrode active layer and a modified matrix layer. The modified matrix layer includes a tubular solid electrolyte body and a modified material layer disposed on the surface of the tubular solid electrolyte body; the modified material layer comprises a conductive polymer. The electrochemical lithium extraction combined with chemical reduction leaching of nickel, cobalt, and manganese using this composite electrode not only achieves high-efficiency recovery of valuable metals such as lithium, nickel, cobalt, and manganese, but also significantly reduces wastewater treatment costs and environmental risks.