Glass plates and pseudo hexagonal prismatic ZSM-5 crystals tethered with 3-aminopropylsilyl (APS) groups, respectively, were prepared by treating them with 3-aminopropyltriethoxysilane. Subsequent treatment of the APS-tethering glass plates with terephthaldicarboxaldehyde led to facile assembly of benzaldehyde (BA) units over the glass plates via imine (–CHN–) linkages. When the BA-tethering glass plates and the APS-tethering zeolite crystals were allowed to contact in boiling toluene, the ZSM-5 crystals strongly adhered onto the glass plates in the form of closely packed monolayers with perfect one-dimensional orientation.