We investigate the extinction coefficients of the surface atmospheric aerosol over the Large High Altitude Air Shower Observatory (LHAASO), located at the Haizi Mountain, Daocheng County, China. To this end, we utilize the Longtin model, Mie scattering theory, and experimental data obtained by the Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observation (CALIPSO). Our theoretical calculations show that the total extinction coefficients of the atmospheric aerosol at the wavelength of 200–500 nm are inversely proportional to the laser wavelength, and influenced by the wind speed. From July 2015 to October 2016, the extinction coefficient of the surface atmospheric aerosols at 532 nm wavelength reached 0.04 km−1 with no wind, while it increased to 0.1 km−1 with gusts. In this period, the extinction coefficients of the surface atmospheric aerosol at 532 nm wavelength, obtained by the CALIPSO, change from 0.01 to 0.07 km−1, which is less than the values obtained the theoretical calculation and larger than the average of Tibetan Plateau in 2006−2016. These calculations and experimental evidence provide important arguments to the model of atmospheric aerosol to be applied in the calibration of LHAASO. Our results suggest that the extinction coefficients over LHAASO require further study, including research on the size distribution, shape, concentration of aerosols particles, wind dependence, relative humidity dependence, etc.