Recently we have trialled the new techniques enabled on Larmor which permit simultaneous measurements of nanoscale and macroscale structure. These experiments gave new insights into the formation of ordered mesoporous silica allowing us to link particle formation and mesostructural ordering processes during growth. Here we wish to apply this combined technique to formation of microcapsules with cellulose nanofibril shells, crosslinked electrostatically or covalently. We aim to follow the crosslinking reactions (which occur over ~12 hrs) in the shells while also monitoring changes in capsule size as the crosslinking occurs. These experiments will allow us to better understand the shell densification and structuring during the crosslinking process to improve our ability to tailor shell properties for encapsulation/release applications of the microcapsules in drug delivery or personal care.