Waterborne polyurethane (WPU) dispersions with a high solid content and low viscosity were prepared successfully by a two-step polymerization with isophorone diisocyanate, poly(propylene glycol), and dimethylol propionic acid as the main raw materials. The molar ratio of hard segments to soft segments was controlled to investigate its influence on the particle size, particle morphology, stability of dispersions, and final properties of the WPU films. Measurements including attenuated total reflectance/Fourier transform infrared spectroscopy, transmission electron microscopy, differential scanning calorimetry, thermogravimetric analysis, Xray diffraction, polarizing optical microscopy, and contact angle tests were used to characterize the bulk structures, phase separation, thermal stability, crystallinity, and wettability of the WPU dispersions. The results indicate that all of the WPU dispersions with a high solid content (ca. 40 wt %) and low viscosity (ca. 20-50 mPa s) displayed excellent stability. The prepared WPU dispersions with acetone contents of 5-7 wt % could be used directly as an ink binder without removing the acetone; this is beneficial to industrial applications of water-based ink binders.WPU is a type of segmented copolymer that consists of hard and soft segments. The hard-segment domains are dispersed in the rubbery soft-segment matrix. The hard segments are commonly formed of diisocyanate and glycol (amine), whereas the soft segments are generally formed of long-chain polyol units. It is known that the hard and soft segments of WPU are distributed in an alternating manner in the polymer structure. 10