The use of nanomaterials for molecular imaging and therapeutics has flourished over the past decade. Controlled assembly and disassembly of nanoparticles is important for applications such as drug delivery systems in order to tune their loading and unloading behavior. Such properties can be accomplished using multivalent non-covalent and porous nanomaterials, such as supramolecular nanoparticles (SNPs) and metal-organic frameworks (MOFs), because of the inherently reversible nature of non-covalent interactions. The main hypothesis investigated in this thesis is whether these, otherwise very different, materials can be controlled in size and outer functionalization according to the same concept, which is the ratiometric variation of multivalent crosslinkers and monovalent stoppers under stoichiometric control.