“…Because of the unique microphase separation behavior, amphiphilic block copolymers (BCPs) have been intensively employed as structure-directing agents for controlled preparation of ordered mesoporous materials over the past decades. − Compared with small amphiphilic molecules (surfactants), BCPs have a series of distinct features, such as adjustable compositions, molecular weights, volume fractions, and molecular architectures, which bring rich mesostructural morphologies through microphase separation and offer a great flexibility in the control of pore size and structure, pore volume, and wall thickness in the development of mesoporous materials. − In this context, the commercially available Pluronic PEO–PPO–PEO block copolymers, including F127, F108, and P123, have been extensively utilized for preparing various mesoporous materials. , Meanwhile, with the development of controllable living polymerization methods, such as atom transfer free radical polymerization (ATRP) and reversible addition–fragmentation chain transfer (RAFT) polymerization, an increasing number of diblock and triblock copolymer systems have been synthesized and employed as soft templates to achieve improved control in the creation of high-quality mesostructured materials with desired structural and composition properties. − For example, various diblock copolymers with hydrophobic blocks containing sp 2 -hybridized carbon have been designed and prepared, − such as poly(ethylene oxide)- block -polyisoprene and poly(ethylene oxide)- block -polystyrene. In relative to commercial Pluronic copolymers, such laboratory-made or tailor-made copolymers possess higher carbon contents as well as higher glass transition temperatures ( T g ) and better thermal stability, making it possible to form well-defined mesostructures with highly crystalline and even single crystalline pore walls. ,− Recently, we also synthesized a new kind of pyrrole-functionalized diblock copolymer [poly(ethylene oxide)- block -poly(6-pyrrol-1-yl-hexyl methacrylate, PEO- b -PPHMA), with which well-defined mesostructured silica, polymer, and carbon materials can be simultaneously constructed .…”