AbstractThe strong electrostatic interactions at the oil–water interface between a small molecule, 5,10,15,20‐tetrakis(4‐sulfonatophenyl)porphyrin, H6TPPS, dissolved in water, and an amine terminated hydrophobic polymer dissolved in oil are shown to produce a supramolecular polymer surfactant (SPS) of H6TPPS at the interface with a binding energy that is sufficiently strong to allow an intermolecular aggregation of the supramolecular polymers. SPSs at the oil–water interface are confirmed by in situ real‐space atomic force microcopy imaging. The assemblies of these aggregates can jam at the interface, opening a novel route to kinetically trap the liquids in non‐equilibrium shapes. The elastic film, comprised of SPSs, wrinkles upon compression, providing a strategy to stabilize liquids in non‐equilibrium shapes.