The activation of both molecules to be oxidized and O2 is critical to accomplish highly efficient catalytic aerobic oxidation under mild conditions,which,however,is very challenging to be achieved and well understood in heterogeneous systems.[1-3] By fabricating sub-5 nm iron nickel hydroxide-platinum hybrid nanoparticles,we demonstrate here a smart,collaborative transition metal-OH-Pt interface that is highly efficient for oxidation catalysis at room temperature.