For the investigation of the correlation between deagglomeration state of primary particles and resulting internal structures as well as mechanical properties of spray-dried granules four SiO2 nanoparticle suspensions were processed differently. An increased milling time results in further deagglomeration and deaggregation of the primary particles within the suspension as well as modified internal structures and increased strengths of the spray-dried granules. The main reason for the higher granule strength can be found in the increasing packing density of the primary particles within the granule shells.