Supported catalysts are widely used in industry and can be optimized by tuning the composition, chemical structure, and interface of the nanoparticle catalyst and oxide support. Here we firstly combine a bottom up colloidal synthesis method with a top down atomic layer deposition (ALD) process to achieve a raspberry-like Pt-decorated Fe3O4 (Fe3O4-Pt) nanoparticle superlattices. This nanocomposite ensures the precision of the catalyst/support interface, improving the catalytic efficiency of the Fe3O4-Pt nanocomposite system. The morphology of the hybrid nanocomposites resulting from different cycles of ALD was monitored by scanning transmission electron microscopy, giving insight into the nucleation and growth mechanism of the ALD process. X-ray photoelectron spectroscopy studies confirm the anticipated electron transfer from Fe3O4 to Pt through the nanocomposite interface. Photocurrent measurement further suggests that Fe3O4 superlattices with controlled decoration of Pt have substantial promise for energy-efficient photoelectrocatalytic oxygen evolution reaction. This work opens a new avenue for designing supported catalyst architectures via precisely controlled decoration of single component superlattices with noble metals.