Traditional cleaning methods can not clean small pollution particles on the surface of cultural relics. Moreover it can easily cause irreversible damage. In order to improve the ability to clean pollutants, laser cleaning technology has been gradually applied to the cleaning of different types of cultural relics. In this paper, we develop a nanosecond laser cleaning system to clean the simulated marble samples and marble fragments in the Palace Museum. The object of the cleanout is black crust pollutants. To avoid the yellowing effect, a dual wavelength combination of 1064 nm near-infrared and 355 nm ultraviolet light is used for laser cleaning of simulated marble samples. When the energy density ratio of these two wavelengths is 3∶2, photos from the microscopic observation system show a good cleaning effect. This ratio (3∶2) is then applied to marble fragments samples. The micro-Raman spectrometer is utilized to evaluate the cleaning effect. The experimental results confirm the advantages of laser cleaning and also provide reference parameters and evaluation methods for laser cleaning of pollutants on marble surface. At the same time, it also offer insights for the application of laser cleaning technology to the cleaning of other stone artifacts.