Architecturally hindered crystallization of bottlebrush graft copolymers offers a reaction- and solvent-free pathway for creating injectable elastomers with tissue-mimetic softness. Currently, injectable materials involve solvents and chemical reactions, leading to uncontrolled swelling, leaching of unreacted moieties, and side reactions with tissue. To address this issue, bottlebrush copolymers with a poly(ethylene glycol) (PEG) amorphous block and crystallizable poly(lactic acid) (PLA) grafted chains (A--B) were synthesized, with grafted chains of controlled length arranged along the backbone at controlled spacing. The densely grafted PEG brush is leveraged to architecturally control both the rate and degree of crystallization of PLA grafts, offering tunability of mechanical properties as a function of architecture and time in a single-component solvent-free system covering a broad range of aggregation states comprising fluid-, paste-, and elastomer-like behaviors with modulus ranging from 1 to 50 kPa. The PLA--PEG pastes are particularly interesting, as they combine solvent-free injectability and time-controlled formation of shape-persistent elastomers at constant temperature. This molecular paste platform may advance reconstructive surgery, drug depots, and tissue engineering.
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