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Supramolecular silicone elastomer is a promising material for sustainable development. Here, quadruple hydrogen bonded ureidopyrimidinone (UPy) units were grafted onto high molecular weight polydimethylsiloxanes (PDMS), providing a novel supramolecular silicone elastomer. The high molecular weight PDMS precursor was prepared through a cyclic trimeric phosphazene base catalyzed ring‐opening polymerization...