Atmospheric aerosols have important impacts on global radiative forcing, air pollution, and human health. This study investigated the optical and physical properties of aerosol layers over Australia from 2007 to 2019 using the Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observations (CALIPSO) Level 2 aerosol products. Australia was divided into three sub-regions (western highlands, central plains, and eastern ranges). Interannual and seasonal optical property variations in aerosol layers in the three sub-regions were analyzed and compared. Results showed that annual mean values of AODL (lowest aerosol layer AOD) and AODT (total AOD of all aerosol layers) were always higher in the eastern ranges region than the other two regions from 2007 to 2019. The reason could be that Australian population was predominantly located in the eastern ranges region, where more human activities could bring significant aerosol loadings. BL (base height of the lowest aerosol layer), HL (top height of the lowest aerosol layer), and HH (top height of the highest aerosol layer) all showed trends of “western highlands > eastern mountains > central plains”, indicating that the higher the elevation, the higher the BL, HL, and HH. TL (thickness of the lowest aerosol layer) was higher during the day than at night, which might account for increased diurnal atmospheric convection and nocturnal aerosol deposition. DRL (depolarization ratio of the lowest aerosol layer) was higher in the western highlands and central plains than the eastern mountains, probably because these two regions have large deserts with more irregularly shaped dust aerosols. CRL (color ratio of the lowest aerosol layer) had slightly higher values in the eastern ranges than the other two regions, probably due to the wet climate of the eastern ranges, where aerosols were more hygroscopic and had larger particle sizes. This study can provide technical support for the control and management of regional air pollutants.