This repository contains the raw data, processed data and python scripts related to the quantitative imaging and modeling of in-operando X-ray micro-computed tomography (µCT) measurements applied to the evaporative drying of silica aerogels. The dataset are linked to two publications (see repository metadata). It also contains the raw data, processed data and python scripts related to the phase composition modeling by wide-angle X-ray scattering (WAXS) measurements reported in the Langmuir publication. The readers are referred to the multiple "README.txt" files for information on the structure of the dataset. Users willing to download the complete dataset should do so by using automated download tools. The reason for that is that Edmond caps any single download at 46.6 GB, and the complete dataset is ~2 TB. This can be done for example with pyDataverse (https://pydataverse.readthedocs.io/en/latest/user/basic-usage.html#download-and-save-a-dataset-to-disk) or using an API (https://guides.dataverse.org/en/latest/api/dataaccess.html#basic-download-by-dataset).