Recently, we have reported successful catalytic reduction of nitro compounds based upon PdPt–Fe₃O₄ heterodimeric nanocrystals as novel magnetically recyclable catalysts. This new catalyst demonstrated the possibility to become an innovative and promising tool for the industrial application in the reduction of nitro compounds with its outstanding advantage such as high efficiency, sustainability and environment-friendliness. Now, we present herein a new one-pot method developed for the selective synthesis of secondary amines via reductive amination of nitriles using the PdPt-Fe₃O₄ catalyst. The PdPt–Fe₃O₄ NPs are very efficient for catalyzing one-pot cascade hydrogenation of a nitro compound and the reductive alkylation of the resulting amine with an imine generated in situ from a nitrile compound. This method allows for the synthesis of unsymmetrical secondary amines with the advantage of avoiding the use of alkyl halides and/or carbonyl compounds. Thus, the new catalytic system offers a highly efficient and useful tool for potential industrial application in the reductive amination reaction of nitriles with nitro compounds.