Aerosol deposition (AD) is a dynamic loading process that can be envisioned as a shock wave loading, necessitating the consideration of the elastic/plastic response of solid materials. Due to the dynamic nature of this process, however, experimental determination of the local pressures during the deposition process is difficult. This work addresses this by investigating the compression and subsequent structure modification of a silicate glass after room‐temperature AD on a silicate glass substrate with Raman spectroscopy. Clear structural changes in the short‐ and middle‐range order of the silicate glass were observed, both as intertetrahedral angle distribution and as ring statistic. Therefore, the AD induced permanent densification of the glass, equivalent, in a hydrostatic approximation, to a minimal pressure of 10.5 ± 1.5 GPa during the film deposition process. Furthermore, the analysis of the Nd3+ photoluminescence of the 4F3/2 − 4I9/2 transition provided complementary information on the glass network modifications occurring during film formation. More than a pure hydrostatic densification, the AD seems to present a very intense shear deformation. This work opens up the perspective of evaluating the mechanical response of film‐substrate and of the particles themselves, and provides critical information on the mechanisms responsible for the AD film formation.