Aqueous polyurethane dispersions based on isophorone diisocyanate (IPDI), poly (tetramethylene adipate) glycol (PTAd), and dimethylolproprionic acid (DMPA) were synthesized by a prepolymer mixing process. Effects of the molecular weight of PTAd and types of hybridizations, viz. blending, semi-interpenetrating polymer network (IPN), and full IPNs with polybutylacrylate have been determined. It was found that thermal, mechanical, and adhesion properties of the polyurethane dispersions increased with increasing molecular weight of polyols. Regarding the effects of hybridization, full IPNs gave the greatest tensile strength and elongation at break with a fast drying rate, whereas semi-IPNs gave the greatest initial as well as final adhesion, implying that a certain degree of chain mobility would augment the penetrations of adhesive molecules into the soft polyurethane foam substrates.