| Summary: | Researchers studying heterogeneous catalysis are intrigued by single-atom catalysts (SACs) due to their ultrahigh atomic utilization. However, only a few reports on SAC-catalyzed classical organic transformations are available. In this work, atomically dispersed Pd sites are confined to a ZrO<sub>2</sub> hybridized N-doped carbon skeleton with a smart design. UiO-66-NH<sub>2</sub> is used to anchor Pd atoms by the coordination of the donor atoms including lone pairs of electrons and metal atoms. Subsequently, the in situ introduction of ZrO<sub>2</sub> doping is achieved using pyrolysis, which helps improve the catalytic performance by modulating the electronic state. The Pd@ZrO<sub>2</sub>/N–C catalyst obtained from the unique design exhibits a high yield (99%) in eco-friendly media with an extremely low noble metal dosage (0.03 mol% Pd) for the Suzuki reaction. Moreover, Pd@ZrO<sub>2</sub>/N–C remains highly active after being reused several times and possesses versatility in a variety of substrates. This strategy offers a feasible alternative to designing SACs with atomically dispersed noble metals for heterogeneous reactions.
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