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Stable emulsions of waterborne polyurethane-acrylic hybrid (WPUA, soft segment content 58.7~58.9 wt%, dimethylol propionic acid: 23.8 mol%/6.6 wt%)/n-butyl acrylate (BA)/methyl methacrylate (MMA)/glycidyl methacrylate (GMA) (weight ratio of BA/MMa/GMA: 4/3/3) hybrid materials containing 20 wt% of acrylic hybrid content were successfully prepared by an emulsifier-/solvent-free prepolmer mixing process. This study examined the effect of butene-1,4-diol/ethylene diamine molar ratio on the stability and viscosity of the hybrid emulsions, the tensile properties/dynamic mechanical thermal properties of hybrid film samples.