Two new uranyl compounds [NH4][(UO2)(ipa)1.5]·H2O 1 and [(UO2)2(μ2OH)(μ3OH)(ipa)(H2O)]·H2O 2 (H2ipa = isophthalic acid) have been synthesized under hydrothermal conditions and characterized by infrared spectra (IR), thermogravimetric analysis (TGA), elemental analyses and X-ray diffraction (XRD). Structural analysis reveals compound 1 exhibits two-dimensional (2D) framework through the bridging of ipa2− anions, which was further construct to three-dimensional (3D) structure via π–π stacking interaction. Compound 2 presents a tetranuclear building block [(UO2)4(μ2OH)2(μ3OH)2(H2O)2] unit which was linked via μ3η4 coordination mode ipa2− anions to form one-dimensional (1D) chains structure. The fluorescence properties of the two compounds were investigated. The photocatalytic performance of compound 2 was also investigated and the results show that compound 2 exhibits good photocatalytic activity toward the degradation of tetracycline antibiotics under LEDs irradiation.