​Our conceived approach based on the directed assembly of functional metal‐organic squares (MOSs), 4‐membered ring (4MR) building units, permitted the construction of two novel zeolite‐like supramolecular assemblies (ZSAs), namely [Co 4 (ImDC) 4 (En) 4 ]·9H 2 O·1.5DMF ( ZSA‐10 ) and [Co 4 (ImDC) 4 (En) 4 ]·7H 2 O ( ZSA‐11 ) (H 3 ImDC = 4,5‐imidazoledicarboxylic acid, En = ethylenediamine, DMF = N,N‐dimethylformamide). The elected MOSs encompass both trans ‐ and cis ‐coordinated nodes, offering complementary peripheral functional groups for their directed assembly into zeolite‐like topologies via supramolecular hydrogen bonding interactions. Distinctly, ZSA‐10 possesses the underling MER zeolite topology and is the only pure MER framework material (without any supporting templates) exhibiting permanent porosity up to now. ZSA‐11 has the underlying ABW topology together with one type of narrow channel.