Methods for treating a substrate are disclosed. The substrate is deoxidized and then immersed in an electrodepositable pretreatment composition comprising a lanthanide series element and/or a Group IIIB metal, an oxidizing agent, and a metal-complexing agent to deposit a coating from the electrodepositable pretreatment composition onto a surface of the substrate. Optionally, the electrodepositable pretreatment composition may comprise a surfactant. A coating from a spontaneously depositable pretreatment composition comprising a Group IIIB and/or Group IVB metal may be deposited on the substrate surface prior to electrodepositing a coating from the electrodepositable pretreatment composition. Following electrodeposition of the electrodepositable pretreatment composition, the substrate optionally may be contacted with a sealing composition comprising phosphate and a Group IIIB and/or IVB metal. Substrates treated according to the methods also are disclosed.