Waterborne polyurethane dispersion (PUD) was synthesized by capping the NCO groups of polyurethane prepolymers, prepared from isophorone diisocyanate, polycarbonate diol and dimethylol propionic acid, with aminopropyl triethoxysilane (APS). Subsequently, silylated acrylic polyurethane dispersion was synthesized by reacting the PUD with the mixture of acrylate monomers, 2-hydroxyethyl methacrylate and methyl methacrylate. The average particle size of silylated acrylic polyurethane dispersion, measured by the dynamic light scattering method, was increased from 39.0 nm to 399.8 nm by increasing the addition amounts of APS. Also, the pencil hardness of coating films of silylated acrylic polyurethane dispersion was enhanced from B grade to F grade with increasing APS content.