The dinuclear SmII complex, [Sm2L4(dme)] (L = OSi(OtBu)3), is easily obtained from the protonolysis reaction of [Sm{N(SiMe3)2}(thf)2] with HOSi(OtBu)3. This complex reacts slowly with toluene, resulting in the isolation of the triple-decker arene-bridged SmII complex, [{Sm2L3}2(μ-η6:η6-C7H8)], in 44% yield. This reactivity provides the first example of unambiguous arene reduction by an isolated SmII species. In contrast, reduction of [SmL3]2 afforded the inverse sandwich complex, [{KSmL3}2(μ-η6:η6-C7H8)].