A new type of supramolecular building block, Zn-II-salpyr [salpyr = N,N'-3-pyridylenebis(salicylideneimine)], is described that contains both a pyridyl donor and a Lewis acidic Zn-II acceptor site in the salen framework. As a consequence, this building block self-organizes into a stable tetrameric vase structure via cooperative intermolecular Zn-N-pyr interactions.