Similarly to what was found for 15 N-py/Ga@SiO2, modelling of experimental 71 Ga NMR data for Ga@SiO2 (SI S6) requires introduction of species that possess a smaller CQ (𝐶 𝑖 𝑄,0 = 15 MHz) than expected from computations (vide supra), as well as a large 𝐶 𝑖 𝑄,0 species, in order to reproduce the lineshape accurately (SI S6), indicating that dynamics may also play a role in decreasing the CQ value of some Ga species present. The sites with lower CQ can be putatively assigned GaBA, where proton dynamics could induce a decrease in CQ, while the sites with significantly higher CQ could be associated with GaLA. However, further analysis would require alternative experimental approaches, such as the use of ultra-high field NMR, to corroborate this assignment, further highlighting the challenges of Ga NMR of high CQ sites.