A regenerated cellulose film (RC) was coated with a graft-IPNs coating, which was composed of castor oil-based polyurethane and 2.8 wt % nitrolignin (NL), to obtain water-resistant films. The effects of NCO/OH molar ratio and different polyols, such as 1,4-butanediol (BDO) and trimethanol propane (TMP), on the structure and properties of the coated RC films were investigated. With an increase of the NCO/OH molar ratio, the tensile strength of the coated films increased, but the water resistivity and size contraction hardly changed. The coated films with TMP exhibited the higher breaking elongation at 1.5 of the NCO/OH molar ratio, while those with BDO have more excellent tensile strength, water resistivity, and dimensional stability. The coated films with the graft-IPNs coating exhibited superior water resistivity and dimensional stability. The light transmittance of the coated films was more excellent than that of the RC film. Moreover, the results from the IR and electron probe microanalysis (EPMA) showed that the chemical bonding occurred between cellulose and coating, and the introduction of NL plays an important role in the enhancement of the interface adhesion of the coated films. Atomic force microscopy (AFM) depicted the flat and dense surface of the coated films, which restricted the water vapor penetration and the size contraction, resulting in the enhancement of water resistivity.