Mesoporous materials are a class of porous materials with pore sizes ranging from 2 to 50 nm. They are distinguished by their high specific surface area, large pore volume, tunable pore size, well-ordered pore channels, and unique confinement effects. As an important class of fundamental materials, mesoporous materials have demonstrated broad application prospects in areas such as energy, catalysis, and drug delivery. To date, the controllable synthesis of mesoporous nanomaterials has been predominantly focused on silica- and polymer/carbon-based systems. However, these materials typically possess single-component frameworks and limited functionalities, making them insufficient to meet the multifunctional demands of complex application scenarios. There is therefore an urgent need to develop novel functional mesoporous nanocomposites by expanding both their framework compositions and composite architectures. This talk will address the key challenges associated with matching and regulating micellar assembly kinetics with framework formation and interfacial assembly kinetics during the synthesis of mesoporous materials. We will highlight a series of newly developed strategies in our group for controlling micelle self-assembly and interfacial assembly, and showcase the resulting new families of mesoporous nanocomposites, including rare-earth-based mesoporous nanocomposites, single-crystalline mesoporous organic–inorganic hybrid materials, and anisotropic mesoporous nanocomposites. The controllable synthesis of these materials substantially broadens the framework components and composite structures of mesoporous nanocomposites, enabling efficient integration and synergistic interactions among multiple functional units, and ultimately enhancing their performance in applications related to disease diagnosis and therapy.