Engineering strong metal–support interactions (SMSI) is an effective strategy for tuning structures and performances of supported metal catalysts but induces poor exposure of active sites. Here, we demonstrate a strong metal–support interaction via a reverse route (SMSIR) by starting from the final morphology of SMSI (fully-encapsulated core–shell structure) to obtain the intermediate state with desirable exposure of metal sites. Using core–shell nanoparticles (NPs) as a building block, the Pd–FeO_xNPs are transformed into a porous yolk–shell structure along with the formation of SMSIR upon treatment under a reductive atmosphere. The final structure, denoted as Pd–Fe₃O₄–H, exhibits excellent catalytic performance in semi-hydrogenation of acetylene with 100% conversion and 85.1% selectivity to ethylene at 80 °C. Detailed electron microscopic and spectroscopic experiments coupled with computational modeling demonstrate that the compelling performance stems from the SMSIR, favoring the formation of surface hydrogen on Pd instead of hydride.