Three volcanic plumes were detected during the Tajogaite volcano eruptive activity (Canary Islands, Spain, September–December 2021) over the Iberian Peninsula. The spatiotemporal evolution of these events is characterised by combining passive satellite remote sensing and ground-based lidar and sun-photometer systems. The inversion algorithm GRASP is used with a suite of ground-based remote sensing instruments such as lidar/ceilometer and sun-photometer from eight sites at different locations throughout the Iberian Peninsula. Satellite observations showed that the volcanic ash plumes remained nearby the Canary Islands covering a mean area of 120 ± 202 km2 during the whole period of eruptive activity and that sulphur dioxide plumes reached the Iberian Peninsula. Remote sensing observations showed that the three events were mainly composed of sulphates, which were transported from the volcano into the free troposphere. The high backscatter-related Ångström exponents for wavelengths 532–1064 nm (1.17 ± 0.20 to 1.40 ± 0.24) and low particle depolarization ratios (0.08 ± 0.02 to 0.09 ± 0.02), measured by the multi-wavelength Raman lidar, hinted at the presence of spherical small particles. The layer aerosol optical depth at 532 nm (AODL532) obtained from lidar measurements contributed between 49% and 82% to the AERONET total column AOD at 532 nm in event II (11–13 October). According to the GRASP retrievals, the layer aerosol optical depth at 440 nm (AODL440) was higher in all sites during event II with values between 0.097 (Badajoz) and 0.233 (Guadiana-UGR) and lower in event III (19–21 October) varying between 0.003 (Granada) and 0.026 (Évora). Compared with the GRASP retrievals of total column AOD at 440 nm, the AODL440 had contributions between 21% and 52% during event II. In the event I (25–28 September), the mean volume concentrations (VC) varied between 5 ± 4 µm3cm-3 (El-Arenosillo/Huelva) and 17 ± 10 µm3cm-3 (Guadiana-UGR), while in event II this variation was from 11 ± 7 µm3cm-3 (Badajoz) to 27 ± 10 µm3cm-3 (Guadiana-UGR). Due to the impact of volcanic events on atmospheric and economic fields, such as radiative forcing and airspace security, a proper characterization is required. This work undertakes it using advanced instrumentation and methods.