Biominerals present in organisms are typically inorganic–organic hybrid materials with unique complex form, hierarchically ordered superstructures, and superior materials properties. Bio‐inspired polymer‐controlled crystallization approaches, aiming to transform the optimized designs and formation mechanisms lurking in biominerals to artificial systems, have been successfully applied to the synthesis of a wide range of inorganic materials. In order to avoid duplication with previous reviews, in this chapter we only focus on the new branches of polymer‐controlled crystallization for the design and preparation of functional inorganic materials with novel structures and improved resulting properties. For clear understanding of the interactions between added polymers and growing crystals and their mediation over the final crystal structures, some basic principles of crystallization involving classical and nonclassical pathways are first introduced. Emphasis will be laid on latest developments and important advances of bio‐inspired synthesis of various kinds of functional inorganic materials via polymer‐controlled crystallization. Their resulting improvements in different properties and potential applications in diverse fields of energy transformation and storage, catalysis, sensing, environmental management, (bio)medical science, and so on are subsequently discussed and highlighted. The challenges of current studies and prospects for future research about this new branch topic are finally suggested.