Castor‐oil‐based anionic PU dispersions are post‐cured using a multiaziridine‐based crosslinker CX‐100. Thermal and mechanical properties of the resulting films are studied by DMA, DSC, TGA, and tensile tests. Mechanical properties are dramatically improved by the crosslinker. For example, the Young's modulus and tensile strength increase from 14.5 to 125 MPa and 13.1 to 18.1 MPa, respectively, when the aziridine fraction increases from 0 to 100%. The onset decomposition temperature of the films, T5, increases from 162 to 209 °C, indicating a significant increase in the thermal stability as the amount of aziridine is increased. This work provides an effective way of curing biorenewable anionic PU dispersions to prepare high performance, environmentally friendly coatings.