A Zn coordination polymer, [Zn(H 2 dhbdc)(Cz-3,6-bpy)] n (1, H 4 dhbdc = 2,5-dihydroxyterephthalic acid, Cz-3,6-bpy = 3,6-bis(pyridin-4-yl)-9Hcarbazole), showing high thermal stability up to 407 °C, has been prepared under hydro(solvo)thermal conditions. Compound 1 has a two-dimensional (2D) undulated layer structure regarded as the topological sql grid, where the tetrahedral Zn(II) centers act as 4-connected nodes connecting by H 2 dhbdc 2− and Cz-3,6-bpy ligands as linkers. Interestingly, the 2D undulated layers expanding in the bc plane are sequentially interwoven with each other in an offset manner along the a-axis, resulting in a condensed polyinterweaving 2D → 3D net. Compound 1 emits weak fluorescence at 522 nm in water suspensions; the intensity can be significantly enhanced by adding Al 3+ ions, with low limit of detection (LOD) of 0.62 μM and high anti-interference ability over numerous competitive metal ions except Fe 3+ ions. Moreover, the detection performance of 1 toward Al 3+ retains high luminescence stability and reusability, being as an excellent candidate for Al 3+ detection over a long period. Spectroscopic evidence from XRPD, EDS, IR, and XPS suggest the occurrence of weak framework−analyte interactions between the H 2 dhbdc 2− ligand units in 1 and the Al 3+ ions, resulting in luminescence turn-on sensing.