Volcanic ash is emitted by most eruptions, sometimes reaching the stratosphere. In addition to its climate effect, ash may have a significant impact on civilian flights. Currently, the horizontal distribution of ash aerosols is quite extensively studied, but not its vertical profile, while of high importance for both applications mentioned. Here, we study the sensitivity of the thermal infrared spectral range to the altitude distribution of volcanic ash, based on similar work that was undertaken on mineral dust. We use measurements by the Infrared Atmospheric Sounding Interferometer (IASI) instruments onboard the MetOp satellite series. The retrieval method that we develop for the ash vertical profile is based on the optimal estimation formalism. This method is applied to study the eruption of the Chilean volcano Puyehue, which started on the 4th of June 2011. The retrieved profiles agree reasonably well with Cloud-Aerosol LiDAR with Orthogonal Polarization (CALIOP) measurements, and our results generally agree with literature studies of the same eruption. The retrieval strategy presented here therefore is very promising for improving our knowledge of the vertical distribution of volcanic ash and obtaining a global 3D ash distribution twice a day. Future improvements of our retrieval strategy are also discussed. © 2016 by the authors.