A method of forming a layered structure comprising a domain pattern of a self-assembled material utilizes a negative-tone patterned photoresist layer comprising non-crosslinked developed photoresist. The developed photoresist is not soluble in an organic casting solvent for a material capable of self-assembly. The developed photoresist is soluble in an aqueous alkaline developer and/or a second organic solvent. A solution comprising the material capable of self-assembly and the organic casting solvent is casted on the patterned photoresist layer. Upon removal of the organic casting solvent, the material self-assembles, thereby forming the layered structure.