This Microreview presents the synthesis of mesoporous, crystalline inorganic materials using self‐assembled block copolymer mesostructures as templates. The advances in this field are discussed in light of the progress in the development of suitable polymer templates. Particular emphasis is placed on the special conditions and demands to transform the primary sol–gel films into mesoporous, aligned crystalline films for functional applications. (© Wiley‐VCH Verlag GmbH & Co. KGaA, 69451 Weinheim, Germany, 2006)