In this work, we attempt to establish a protocol using rapidly computed data to allow efficient forecasting of integrative self-assembly of ligands to form heteroleptic MOCs. To achieve this goal, the self-assembly of binary combinations of ditopic ligands with Pd(II) ions was examined experimentally. From the twelve possible ligand combinations, two pairs were observed to cleanly form heteroleptic cis-Pd2L2L'2 cages. A hierarchy of calculations of varying computational expense were then used to rationalise the self-assembly outcomes. While ligand-based approaches proved effective in mirroring experimental data, cage-based analyses uncovered limitations in the modelling process of great importance for the computationally-aided design of MOCs.