High entropy alloys (HEAs) are promising heterocatalysts because of their unique physicochemical properties, but research on HEA‐catalyzed tandem reactions is lacking. Moreover, limited research on HEAs for molecular transformation has hindered their development. Herein, an unsupported nanoporous HEA Al‐Pt‐Pd‐Ru (HEANPore) prepared using a top‐down dealloying method is reported. The Lewis acidity and electron redistribution of the noble metals Pt, Pd, and Ru are identified to be intrinsic of high activity and selectivity of HEANPore in the one‐pot reductive amination of nitroarenes. The competitive adsorption of the reactant and corresponding reaction mechanism are investigated using DFT. This study demonstrates the exceptional performance of the HEANPore in tandem reactions, presenting new possibilities for the application of HEAs in the field of catalysis.