Seven new isostructural lanthanide metal-organic frameworks (Ln-MOFs), [Ln(Hpzbc)(2)(NO3)]center dot H2O (1-Ln, Ln = Nd3+, Sm3+, Eu3+, Gd3+, Tb3+, Er3+, and Yb3+ ions, H(2)pzbc = 3-(1H-pyrazol-3-yl) benzoic acid), with one-dimensional (1D) channels decorated by nitrate anions and pyrazoyl groups have been constructed. 1-Ln, as revealed by structural analysis, represent uncommon microporous 3D Ln-pyrazoyl-carboxyl systems using pyrazoyl-carboxyl bifunctional ligands as bridges. The luminescent investigations show that 1-Eu is an excellent MOF-based fluorescent probe, with high sensitivity, selectivity, and simple regeneration, for environmentally relevant Fe3+ and Cr2O72- ions. 1-Eu also presents highly selective capture for CO2 over N-2 and CH4 due to the multiple binding sites for CO2 molecules, which were supported by Grand Canonical Monte Carlo (GCMC) simulations.