The cellular Yule-Nielson spectral Neugebauer (CYNSN) model to characterize a typical CMYK (i.e., cyan, magenta, yellow, and black) 4-ink color printer is presented. By reconstructing spectral reflectance, models with high accuracy of spectral and colorimetric predictions are built. A novel cell-searching algorithm is proposed and used together with the iteration method to invert the cellular Neugebauer model efficiently. Large numbers of high quality hardcopy samples are produced to evaluate model performance and prove the feasibility of the algorithm. The spectral-based model performs better compared with the usual model based on CIE1931 XYZ tristimulus values.