We present two case studies of tropospheric aerosol transport observed over the high-altitude Helmos observatory (1800–2300 m a.s.l.) in Greece during September 2021. Two cases were linked to Saharan dust intrusions, of which one was additionally linked to a mixture of biomass-burning and continental aerosols. Aerosol vertical profiles from the AIAS mobile backscatter/depolarization lidar (532 nm, NTUA) revealed distinct aerosol layers between 2 and 6 km a.s.l., with particle linear depolarization ratio values of up to 0.30–0.40, indicative of mineral dust. The elevated location of Helmos allows lidar measurements in the free troposphere, minimizing planetary boundary layer influence and improving the attribution of long-range transported aerosols. Radiative impacts were quantified using the LibRadtran model. For the 27 September dust outbreak, simulations showed strong shortwave absorption within 3–7 km, peaking at 5–6 km, with surface forcing reaching −25 W m−2 and TOA forcing around −12 W m−2, thus, implying a net cooling by 13 W m−2 on the Earth’s atmosphere system. In contrast, the 30 September mixed aerosol case produced substantial solar attenuation, a surface heating rate of 2.57 K day−1, and a small positive forcing aloft (~0.05 K day−1). These results emphasize the contrasting radiative roles of dust and smoke over the Mediterranean and the importance of high-altitude observatories for constraining aerosol–radiation interactions.