It is an attractive but challenging proposition to develop effective fluorescent sensors for detecting specific organic compounds. In this study, we designed and synthesized three Zn(II) complexes, namely [Zn(3N3PY)(2)](NO3)(2)center dot 3.5CH(3)OH (1), [Zn(3N3PY)(BIN)]center dot 1.5DMF (2) and [Zn(3N3PY)(BIN)(0.5)(HCOO)) (3) (H2BIN = 2,2'-biisonicotinic acid, HCOO- = formate), using a D-pi-A ligand 4'-(4-(1H-1,2,4-triazol-1-yl)phenyl)2,2':6',2 ''-terpyridine (3N3PY) with mononuclear, one-dimensional (1D) chain and dinuclear structures, respectively. The three-dimensional (3D) supramolecular assemblies were achieved by the linkage of the Zn(II) complexes through pi-pi and hydrogen bonding interactions. The assemblies demonstrated intense luminescence and exhibited an excellent ability for sensing specific organic molecules namely 2,4,6-trinitrophenol (TNP), 4-methylbenzaldehyde (4-MB) and decabromodiphenyl oxide (DBDPO).