Atmospheric correction is a necessary step for deriving surface geophysical parameters. The aim of this paper is to study the atmospheric correction of Landsat-8 imageries released by the Institute of Remote Sensing and Digital Earth, Chinese Academy of Sciences. A look-up table (LUT)-based atmospheric correction method on Landsat-8 OLI is proposed. The LUT is generated with 6S model with inputs including total atmospheric water vapor content, ozone, and aerosol optical thickness (AOT) from MODIS atmospheric level 2 products. The conventional method to build up the atmospheric parameter LUT usually only takes part of the factors (e.g., AOT) into consideration, whereas it is not applicable in the atmospheric correction using per pixel of MODIS products as input atmospheric parameters. Thus, a five-dimensional LUT, which considers most input parameters, is built up and has high universality for the Landsat-8 OLI sensor. Finally, spectral analysis, comparison to U.S. Geological Survey-released surface reflectance (SR) products, and field observations are used to validate the quality of the model-computed SR. The validation results indicate that the proposed method can effectively generate accurate and reliable SR results, although there is an overcorrected problem in the costal blue region when the AOT value is very high.