Having demonstrated that our phase space contains most of the structures spanned by the ordered, enantiopure, desolvated octahedral cages, the natural question is, given a novel cage, can we predict its likely solid-state structure using our simulations? And what design rules can we assimilate from our coarse-grained model? For the former, in order to gain insight of the most dominant packing types (e.g. windowto-arene) and likely value of σ ang , a process must be created to relate the interactions between cages, as calculated through atomistic methods, to our phase space. Although density functional theory (DFT) dimer pair calculations examining packing motifs have proven to be deterministic of preferred packing behaviour, 10 establishing a robust relationship between DFT results and a continuous parameter such as σ ang is a more complex task. We have started to address this problem by examining the energetics of two cages slipping around the central patch position (see Section S7). The goal here is to relate the energies produced from atomistic calculations to the parameters of our model, creating a relationship between each region of our phase space to a range of interaction energies. Therefore, by using this relationship for novel cages, we can use atomistic simulations of two cage molecules to extrapolate to solid-state, crystalline phase behaviour. However, for both the window-to-window and window-to-arene simulations there are only two desolvated cages that have been reported to form any of the predicted crystal structures: (i) CC9-R3 and CC1β ′ in the window-to-arene simulations, (ii) CC3α and CC4β in the window-to-window simulations. Moreover, the predicted crystal structures are found in a narrow, if not the same, region of phase space.