LAUSR

Owing to their highly predictable porous structures, facile synthesis, and the presence of functional open metal sites, metal–organic frameworks (MOFs) are extensively employed in various fields, including energy storage, catalysis, adsorption, and separation. Nevertheless, the limited hydrolytic stability exhibited by numerous MOFs poses a significant challenge to their practical application. In the present study, we present the synthesis and characterization of a uranyl organic framework (TCPP‐U1) with a highly porous structure, which is constructed by assembling cobalt, uranyl, and the porphyrin ligand 5,10,15,20‐tetra(4‐carboxyphenyl)porphyrin (TCPP). However, TCPP‐U1 demonstrates poor hydrolytic stability when exposed to water (the structure can be destroyed even after 2 min of exposure to water), greatly impeding its potential applications that would benefit from its high surface area. To address this limitation, we developed a hybrid composite by incorporating acid‐treated multi‐walled carbon nanotubes (CNTs) into the TCPP‐U1 framework via a solvothermal method designated as CNTs@TCPP‐U1. Remarkably, the obtained CNTs@TCPP‐U1 composite possesses an identical crystal structure and morphology to the original TCPP‐U1 yet exhibits significant enhancements in hydrolytic stability (the structure remains stable even after 3 days of immersion in water). Furthermore, CNTs@TCPP‐U1 demonstrates a significant photocatalytic effect on the degradation of tetracycline hydrochloride in aqueous solutions. The reaction rate constant (k) for the pseudo‐first‐order kinetic model is 0.0059 min−1. Our findings present a novel perspective for enhancing the stability and expanding the performance of MOFs materials.