Bradley F. Chmelka

Inorganic–organic mesophase materials provide a wide range of tunable properties, which are often highly dependent on their nano‐, micro‐, or meso‐scale compositions and structures. Among these are macroscopic orientational order and corresponding anisotropic material properties, the adjustability of which are difficult to achieve. This is due to the complicated transient and coupled transport, chemical reaction, and surface processes that occur during material syntheses. By understanding such processes, general criteria are established and used to prepare diverse mesostructured materials with highly aligned channels with uniform nanometer dimensions and controllable directionalities over macroscopic dimensions and thicknesses. This is achieved by using a micropatterned semipermeable poly(dimethylsiloxane) stamp to manage the rates, directions, and surfaces at which self‐assembling phases nucleate and the directions that they grow. This enables mesostructured surfactant‐directed silica and titania composites, including with functional guest species, and mesoporous carbons to be prepared with high degrees of hexagonal order, as well as controllable orthogonal macroscopic orientational order. The resulting materials exhibit novel anisotropic properties, as demonstrated by the example of direction‐dependent photocurrent generation, and are promising for enhancing the functionality of inorganic–organic nanocomposite materials in separations, catalysis, and energy conversion applications.