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In this study, core‐shell structured cationic waterborne polyurethane (WPU) dispersions with high solid content were prepared. To this end, prepolymer A was synthesized from polytetramethylene ether glycol (PTMG), isophorone diisocyanate (IPDI), castor oil (CO) and 1,4‐butanediol (BDO) without integration of the hydrophilic groups. Prepolymer B with hydrophilic groups was prepared from PTMG, IPDI, CO, BDO and N‐methyldiethanol amine (MDEA). WPU dispersion with a core‐shell structure could be generated by mixing, neutralizing, and emulsifying of the prepolymer A and the prepolymer B. The results indicated that the generation of WPU dispersions through this technique exhibited a milky appearance while the pH values range from 5.30 to 5.60. The optimal combination of prepolymer A and prepolymer B (at a ratio of 5:5) resulted in a dispersion with the highest solid content (50.4%), lowest viscosity (69 mPa·s), and narrowest particle size distribution. As the proportion of prepolymer A to prepolymer B decreases, the tensile strength of WPU film reduces while the elongation at break and glass transition temperature increases. Moreover, initially the contact angle with water was decreased instead of increase. However, modifications in a ratio of prepolymer A and B was not showed any significant impact on the thermal stability performance of the WPU films. [ABSTRACT FROM AUTHOR]