Here, 𝜙 describes the preference for incorporation of polymer-bound bis-pyridine ligands into MOC structures and is equal to the fraction of L1 moieties in MOC structures divided by the fraction of all ligand moieties in the mixture that are L1. We derived the following inequality which predicts gelation to occur when: provide a general framework for the design of stimuli-responsive materials via guest-biding within tailor-made nested MOC cavities in general.