Five new metal−organic frameworks, [Zn 2 L 2 ]·2DMF·2MeOH (1), [Zn 2 L 2 (py) 2 ] (2), [Cd 2 L 2 ]·Diox·MeOH·6H 2 O (3), [Mn 2 L 2 ]·2DMF·2MeOH (4), and [Co 2 L 2 ]·2DMF·4H 2 O (5), were assembled by using a novel 8-hydroxyquinolinatederivative H 2 L with different metal ions. Complex 1 features a 3Dporous network consisting of meso-helical chains (P + M) built frommetal−ligand coordination bonds. The adjacent dinuclear Zn IIbuilding blocks in 2 are connected together to generate a 2D gridnetwork. In complex 3, each binuclear motif is bound to four Zn IIions to produce a 2D layer structure that stacks into a 3D porousstructure. The framework of complex 4 is isostructural to 5, featuringa 2 1 helical chain built from [M 2 L 2 ] units (M = Mn or Co). Theadjacent meso-helices associated in parallel are interconnected by thephenolate μ 2 -O atoms of H 2 L to give rise to a 2D network. Distinctsolid-state luminescence properties of 1−3 were observed, arising from their different metal nodes and frameworks. Inparticular, complex 1 exhibited excellent stability in both common organic solvents and H 2 O, thus facilitating its utility as achemical sensor. Remarkably, luminescent 1 showed highly sensitive detection for nitroaromatic molecules in methanol andFe 3+ ion in H 2 O even in the presence of other interfering metal cations.