The present invention provides articles and methods for affecting the self-assembly of materials. In some cases, the invention provides an approach for facilitating the self-assembly of various materials, including polymeric materials (e.g., block polymers), nanoparticles, other materials capable of self-assembly, and the like, over relatively large surface areas. Some embodiments of the invention provide articles (e.g., substrates) which, when contacted with a material capable of self-assembly, may produce greater control of self-assembly through the bulk of the material.