The synthesis and thermomechanical properties of a novel class of self-healing perfluoropolyethers (PFPEs) is reported. By decoration of 2-ureido-4[1H]-pyrimidone end groups on the termini of low molar mass PFPE, the formation of supramolecular polymers and networks held together via hydrogen bonding associations was achieved. These novel supramolecular polymer materials exhibit a combination of enhanced modulus and elasticity, along with self-healing properties, where rapid self-healing time was demonstrated using dynamic rheological measurements. These types of supramolecular PFPEs are anticipated to be useful for a number of emerging areas in lubrication. (c) 2013 Wiley Periodicals, Inc. J. Polym. Sci., Part A: Polym. Chem. 2013, 51, 3598-3606