Abstract Mechanochemical approaches are widely used for the efficient, solvent‐free synthesis of organic molecules, however their applicability to the synthesis of functional polymers has remained underexplored. Herein, we demonstrate for the first time that mechanochemically triggered free‐radical polymerization allows solvent‐ and initiator‐free syntheses of structurally and morphologically well‐defined complex functional macromolecular architectures, namely stimuliresponsive microgels. The developed mechanochemical polymerization approach is applicable to a variety of monomers and allows synthesizing microgels with tunable chemical structure, variable size, controlled number of crosslinks and reactive functional end‐groups.
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