We report an original catalytic molecular tetrahedron. By threading through the cavity of the tetrahedron, polymeric substrates are unfolded or broken apart. Our catalyst distinguishes between polymer chains of different lengths, functionalizing the shorter polymers selectively over the longer ones-as a proof of concept for selective catalysis to modify polymers. Our findings advance the fundamental understanding of the thermodynamic and kinetic phenomena controlling the interactions between molecular cages and synthetic polymers, offering valuable ability to create complex materials in the future.

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