A workpiece including aluminum or an aluminum alloy on a surface thereof is subjected to surface treatment including the steps of immersing in an acidic or alkaline aluminum oxide film-removing solution containing a salt or oxide of a metal capable of substitution with aluminum and forming a substituted metal layer and contained in the removing solution on a surface of the aluminum or aluminum alloy while removing an aluminum oxide film on aluminum or aluminum alloy surface, forming a substituted zinc film by zinc substitution treatment without removing the substituted metal layer, removing the substituted metal layer and substituted zinc film with an oxidizing liquid, and subjecting again to zinc substitution treatment, forming a substituted zinc film.