The metal–arene interactions motivated the advancement of chemical bond theory, and enabled a wide range of applications in synthesis and catalysis. In addition, ligand designs incorporating metal–arene interaction led to breakthroughs in stabilizing unusual oxidation states, and empowering small molecule activation and catalysis. Our group focuses on utilizing f-block metal-arene interactions in synthesis and catalysis. We have synthesized a series of inverse-sandwich f-block metal arene complexes and explored their reactivity.^[1,2,3] Moreover, we have incorporated metal-arene interaction in ligand design and developed tripodal tris(amino)arene ligands.^[4] We showed that this type of ligand is able to not only support multiple oxidation states of f-block metals,^[5] but also enable unprecedented redox chemistry at the metal site.^[6] Our results unveiled that the f-block metal-arene interaction can induce dual reactivity of metal and arene.