<p>Herein, we developed a Pd/UiO-66-NO catalyst for the reductive amination of benzaldehyde with aniline to synthesize <i>N</i>-benzylaniline. Through post-synthetic modification, salicylaldehyde was incorporated into the UiO-66-NH₂ framework to construct a support (UiO-66-NO) featuring N, O-bidentate chelating sites, which enabled the stabilization of highly dispersed Pd nanoparticles. Characterization results confirmed the preserved framework integrity and demonstrated efficient secondary amine synthesis under mild conditions (60&#xa0;°C, 3&#xa0;h). The catalyst exhibited broad substrate scope with excellent functional group compatibility. Mechanistic studies revealed a two-step pathway involving amine-aldehyde condensation followed by hydrogenation of the imine intermediate. ¹H NMR and GC kinetic analyses evidenced rapid imine formation and subsequent efficient reduction to the secondary amine. This study provides a new strategy for designing high-performance heterogeneous catalysts and opens up a viable pathway for the efficient synthesis of secondary amines.</p> Graphical Abstract <p></p>