The work presents the first example of employing a template group in a bifunctional ligand to construct an infinite polypseudorotaxane, in which 2D undulated sql anionic sheets are penetrated by 1D linear cationic chains. The bifunctional ligand also leads to the formation of an unprecedented 3D (3,4,4)-connected network with {4.72}2{4.73.8.9}2{72.93.11} topology.
