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<p>The spatiotemporal distributions of aerosol optical properties and major aerosol types, along with the vertical distribution of major aerosol types over Australia, are investigated based on multi-year Aerosol Robotic Network (AERONET) observations at nine sites, the Moderate Resolution Imaging Spectroradiometer (MODIS), Modern-Era Retrospective analysis for Research and Applications, Version 2 (MERRA-2), Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP), and back-trajectory analysis from the Hybrid Single-Particle Lagrangian Integrated Trajectory (HYSPLIT). During the observation period from 2001–2020, the annual aerosol optical depth (AOD) at most sites showed increasing trends (0.002–0.029 yr<span class="inline-formula">⁻¹</span>), except for that at three sites, Canberra, Jabiru, and Lake Argyle, which showed decreasing trends (<span class="inline-formula">−</span>0.004 to <span class="inline-formula">−</span>0.014 yr<span class="inline-formula">⁻¹</span>). In contrast, the annual Ångström exponent (AE) showed decreasing tendencies at most sites (<span class="inline-formula">−</span>0.045 to <span class="inline-formula">−</span>0.005 yr<span class="inline-formula">⁻¹</span>). The results showed strong seasonal variations in AOD, with high values in the austral spring and summer and relatively low values in the austral fall and winter, and weak seasonal variations in AE, with the highest mean values in the austral spring at most sites. Monthly average AOD increases from August to December or the following January and decreases during March–July. Spatially, the MODIS AOD showed obvious spatial heterogeneity, with high values appearing over the Australian tropical savanna regions, Lake Eyre Basin, and southeastern regions of Australia, while low values appeared over the arid regions in western Australia. MERRA-2 showed that carbonaceous aerosol over northern Australia, dust over central Australia, sulfate over densely populated northwestern and southeastern Australia, and sea salt over Australian coastal regions are the major types of atmospheric aerosols. The nine ground-based AERONET sites over Australia showed that the mixed type of aerosols (biomass burning and dust) is dominant in all seasons. Moreover, Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observations (CALIPSO) showed that polluted dust is the dominant aerosol type detected at heights 0.5–5 km over the Australian continent during all seasons. The results suggested that Australian aerosol has similar source characteristics due to the regional transport over Australia, especially for biomass burning and dust aerosols. However, the dust-prone characteristic of aerosol is more prominent over central Australia, while the biomass-burning-prone characteristic of aerosol is more prominent in northern Australia.</p>