Catalyst systems with high catalytic activity and sustainability are highly desirable. Here, we report a design for catalytic composites with a hierarchical structure in which polydopamine (PD), multi-metallic nanocatalysts and iron oxide nanoneedles are successively deposited on a magnetic core. PD layers with various thicknesses are coated onto the magnetic core and serve as a template by which to take up multi-metallic nanocatalysts such as Au, Ag and Pt nanoparticles. The iron oxide nanoneedles act as spacers, preventing the nanocomposite from aggregating and increasing the surface area of the composite. The distinctive structures of the controllable template, the multi-metallic catalysts and needle-like layers enable the rapid migration of reactive ionic species and enhance catalytic ability via the synergistic effect of the multi-metallic nanocatalysts and iron oxide nanoneedles. Moreover, due to the strong magnetic property of the catalytic nanocomposites, they can be easily recovered with an external magnet and reused. Our hierarchical nanocomposites for recyclable nanocatalysts provide a new design concept for highly efficient catalysts.