Monolayered adatom aggregation induced by metallofullerene molecules on Cu(100)

► The adsorption and self-assembly of Gd@C82 molecules on Cu(100) were studied by STM. ► The formation of Cu monolayer islands underneath Gd@C82 molecules was revealed. ► The Cu adatoms aggregated upon adatom-metallofullerene complexation. ► The assembled molecules show orientational ordering, agreeing with DFT calculation.