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In many sensing and catalytic applications, the target molecule is required to be carried in an effective manner in a specific condition. Metal-organic frameworks (MOFs) have high porosity, large surface area, and tunable functionality and are promising carriers for such purposes. Current approaches to detect Tb3+ and reduce 4-nitrophenol (4-NP) are based on multistep methods. We synthesized a series of coordination polymers (1-4) with excellent fluorescence and catalytic activity. Moreover, 1 and 2 exhibit significantly higher fluorescence than other compounds, indicating that 1 and 2 could be efficient multifunctional fluorescence probes for high-sensitivity sensing of nitrobenzene, and 1 can be used as a highly sensitive fluorescent sensor to detect Tb3+, with a detection limitation of 5 × 10−7 M. In addition, the as-prepared Ag@compound 1 shows remarkable catalytic performance to reduce 4-NP, with a reduction rate constant k as large as 2.07 × 10−2 s−1. [ABSTRACT FROM AUTHOR]