AbstractAnodization was employed to treat the aluminum foil surface, leading to in situ the generation of Al2O3, consequently amplifying the specific surface area to aid in the dispersal of palladium nanoparticles. Through the anodic oxidation of aluminum followed by a precipitation‐deposition and calcination process, a highly efficient and reusable Pd/Al2O3/Al monolithic catalyst was synthesized. The effectiveness and reusability of the Pd/Al2O3/Al monolithic catalyst were evaluated in the Suzuki‐Miyaura reaction. The turnover number (TON) and turnover frequency (TOF) of the Pd/Al2O3/Al monolithic catalyst reached 73,880 and 0.86 s−1, respectively. Furthermore, the catalyst could be recovered and reused in reactions regardless of the used substrates.