Self-assembly is an effective strategy for the creation of periodic structures at the nanoscale. However, because microelectronic devices use free-form design principles, the insertion point of self-assembling materials into existing nanomanufacturing processes is unclear. We directed ternary blends of diblock copolymers and homopolymers that naturally form periodic arrays to assemble into nonregular device-oriented structures on chemically nanopatterned substrates. Redistribution of homopolymer facilitates the defect-free assembly in locations where the domain dimensions deviate substantially from those formed in the bulk. The ability to pattern nonregular structures using self-assembling materials creates new opportunities for nanoscale manufacturing.