The volcanic eruption of Cumbre Vieja (La Palma Island, Spain), started on 19 September 2021 and was declared terminated on 25 December 2021. A complete set of aerosol measurements were deployed around the volcano within the first month of the eruptive activity. This paper describes the results of the observations made at Tazacorte on the west bank of the island where a polarized micro-pulse lidar was deployed. The analyzed two-and-a-half months (16 October–31 December) reveal that the peak height of the lowermost and strongest volcanic plume did not exceed 3 km (the mean of the hourly values is 1.43 ± 0.45 km over the whole period) and was highly variable. The peak height of the lowermost volcanic plume steadily increased until week 11 after the eruption started (and 3 weeks before its end) and started decreasing afterward. The ash mass concentration was assessed with a method based on the polarization capability of the instrument. Two days with a high ash load were selected: The ash backscatter coefficient, aerosol optical depth, and the volume and particle depolarization ratios were, respectively, 3.6 (2.4) Mm−1sr−1, 0.52 (0.19), 0.13 (0.07) and 0.23 (0.13) on 18 October (15 November). Considering the limitation of current remote sensing techniques to detect large-to-giant particles, the ash mass concentration on the day with the highest ash load (18 October) was estimated to have peaked in the range of 800–3200 μg m−3 in the lowermost layer below 2.5 km.