The present invention provides continuous, free-standing metal oxide films and methods for making said films. The methods are able to produce large-area, flexible, thin films having one or more continuous, single-crystalline metal oxide domains. The methods include the steps of forming a surfactant monolayer at the surface of an aqueous solution, wherein the headgroups of the surfactant molecules provide a metal oxide film growth template. When metal ions in the aqueous solution are exposed to the metal oxide film growth template in the presence of hydroxide ions under suitable conditions, a continuous, free-standing metal oxide film can be grown from the film growth template downward into the aqueous solution.