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We fabricate soft, solvent-free polydimethylsiloxane (PDMS) elastomers by crosslinking bottlebrush polymers rather than linear polymers. We design the chemistry to allow commercially available linear PDMS precursors to deterministically form bottlebrush polymers, which are simultaneously crosslinked, enabling a one-step synthesis. The bottlebrush architecture prevents the formation of entanglements, resulting in elastomers with precisely controllable elastic moduli from ~1 to ~100 kPa, belowdoi:10.17615/zac9-ct04 fatcat:krcidqmve5antihgr2eeh6njcm