Polyurethane (PU) prepolymers are prepared by a polyaddition of isophorone diisocyanate, polypropylene glycol-1000, and 2,2-dimethylolpropanic acid. The anionic aqueous-based PU dispersions are derived from a water dispersion process of these NCO-terminated PU prepolymers together with a neutralization and a chain extension. They have both terminal amino and pendent carboxylic groups which are potentially reactive sites toward a di-functional epoxy and a tri-or di-aziridinyl compound of a dual-curing PU system, respectively. The stabilities of the resulting PU dispersions on zeta potential and particle size distributions are investigated. The improvements on mechanical, physical, and thermal properties of these dual-cured PU systems are also evaluated.