A metal surface treatment composition including at least one compound selected from the group consisting of a zirconium compound and a titanium compound, and an organosiloxane, which is a polycondensate of organosilane and has in a molecule thereof of at least two amino groups, in which the Degree of polycondensation of the organosiloxane is at least 40%, the content of at least one compound selected from the group consisting of the zirconium compound and the titanium compound is predetermined content, the content of the organosiloxane in the metal surface treatment composition is predetermined content, and the mass ratio of at least one element selected from the group consisting of the zirconium element and the titanium element contained in the zirconium compound and the titanium compound, respectively, to the silicon element contained in the organosiloxane is a predetermined ratio.