To better understand the structural outcomes identified in the screen using the automated analysis, computational modelling was performed on the MNLN (where N = 4 or 12) and M2X3 (where X = L or I) structures, details of which are given in Supporting Information Section S4. First, the M4L4 tetrahedra were modelled at a semi-empirical level (Figure ), with a T-symmetric configuration. For both triamines A and B, the MOCs assembled with the methyl-substituted pyridyl aldehydes 2, 3, and 4 are isomers of each other, and therefore the relative energies for the different tetrahedra can therefore be compared (Table ).