Diaminotriazine-functionalized polystyrene folds into a highly compact micelle-like structure in nonpolar solvents, as established by gel permeation chromatography. Folding of this polymer arises from intramolecular hydrogen bonding between the triazine moieties, allowing the unfolding process to be effected through competitive intermolecular host-guest interactions. Variable-temperature NMR titrations of this polymer with a complementary host were used to quantify the thermodynamics of this unfolding process.