The Kubelka-Munk (K-M) theory combined with the mixing theory has been successively applied to the color prediction of colorant such as paints, dyes and printing inks with fine colored particles. Limited by ancient grinding and sieving technology or for intended use, the mineral pigments used in colored relics usually have a relatively larger particle size. This work investigates the spectrophotometric color prediction of mineral pigments with large particle size by applying the single- and twoconstant K-M theory. Results indicate that (a) one sample (i.e., a tint with 80% colored and 20% white mineral pigment) and two samples (i.e., a masstone and a tint with 40%-60% colored mineral pigment) are sufficient to characterize the optical constants of the colored mineral pigment for single- and twoconstant K-M theory respectively, and (b) that two-constant K-M theory has a significantly higher prediction accuracy due to the specific particle size and film formation mechanism of the mineral pigments.