Acrylic terminated polyurethane prepolymers were synthesized by capping the NCO groups of polyurethane prepolymers, prepared from isophorone diisocyanate (IPDI), polycarbonate diol (PCD) and dimethylol propionic acid (DMPA), with pentaerythritol triacrylate (PETA). Subsequently, silylated acrylic terminated prepolymers were prepared by capping the NCO groups of acrylic terminated polyurethane prepolymers with different types of silane coupling agents, glycidoxypropyl trimethoxysilane (GPTMS) or aminopropyl triethoxysilane (APS). The average particle size of pure waterborne polyurethane solution, measured by the dynamic light scattering method, was increased from 14.3 nm to 208.6 nm by adding PETA and APS. Also, the coating film of silylated acrylic terminated waterborne polyurethane showed better abrasion resistance and pencil hardness than that of pure waterborne polyurethane.