This work reports a facile one-step method for the fabricating Fe3O4@Au/polydopamine sandwich-like core-shell nanostructure, in which the Au/polydopamine (Au/PDA) hybrid shell is obtained via an in situ redox-oxidation polymerization between the HAuCl4 and dopamine. The content of Au nanocrystals, shell thickness, and particle sizes are tunable by varying the experimental parameters. Intriguingly, this general method can be applied for different functional nanostructures such as the β-FeOOH@Au/PDA, SiO2@Au/PDA, and CNT@Au/PDA nanocomposites. A possible formation mechanism is proposed and it is found that the surface interaction plays a key role in determining the final nanostructure. The as-prepared Fe3O4@Au/PDA exhibited eminent catalytic activity on the reduction of 4-nitrophenol. Since the external PDA shell prevents the Au nanocrystals from leaching during the reduction, the cycling activity has been maintained as high as 95% after seven times of catalytic reaction.