Two different diene monomers [dicyclopentadiene (DCPD) and 5-ethylidene-2-norbornene (ENB)] as self-healing agents for polymeric composites were microencapsuled by in situ polymerization of urea and formaldehyde. We obtained plots of the storage modulus (G') and tan δ as a function of cure time by using dynamic mechanical analysis to investigate the cure behavior of the unreacted self-healing agent mixture in the presence of a catalyst. Glass transition temperatures (T_g) and exothermic reactions of samples cured for 5 and 120 min in the presence of different amounts of the catalyst were analyzed by differential scanning calorimetry. Of the two dienes, ENB may have advantages as a self-healing agent because, when cured under same conditions as DCPD, it reacts much faster in the presence of a much lower amount of catalyst, has no melting point, and produces a resin that has a higher value of T_g. Microcapsules containing the healing agent were successfully formed from both of the diene monomers and were characterized by thermogravimetric analysis. Optical microscopy and a particle size analyzer were employed to observe the morphology and size distribution, respectively, of the microcapsules. The microcapsules exhibited similar thermal properties as well as particle shapes and sizes.