The scrambled cages were soaked in MeOH to exchange out the DMA molecules prior to activation and gas sorption measurements. All samples were characterised via IR spectroscopy, PXRD, TGA, and 1 H-NMR spectroscopy of digested samples, with the data presented in the SI. IR spectra of the samples (Fig. ) show that characteristic stretching vibration highlighted in Fig. (a) are still present in all of the corresponding cages with their relative intensities unchanged, suggesting that the composition of the cages is unaltered after solvent exchange. The 1 H-NMR spectra (Fig. ) of aciddigested samples confirm that the composition of the cages in terms of the ligand ratios remains the same, with successful exchange of DMA for MeOH taking place, while the TGA data show that the overall thermal stability of the cages is unaltered. The PXRD data for [Cu4(L)4-x(CH3L)x]-MeOH show that as x increases, the crystallinity of the bulk powder also increases (Fig. ). A similar, although less pronounced, effect is also observed for the family [Cu4(MeOL)4-x(CH3L)x]-MeOH (Fig. ), although the overall effect of the methoxy substituent appears to be a reduction in the crystallinity of this family of cages compared to the family [Cu4(L)4-x(CH3L)x].