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A series of metallocene complexes [Ln{η⁵:σ-Me₂C(C₅H₄)(C₂B₁₀H₁₀)}₂][Li(DME)₃] (1Ln) (Ln = Tb, Dy, Ho, Er) were prepared with both σ-Cp and π-Cp interactions included. Based on 1Ln, a heteroleptic sandwich SMM [2-THF-2'-(μ²-Cl)Li(THF)₃-2,2'-Ln(nido-1,7-C₂B₉H₁₁)Cp*] (2Dy) was synthesized, exhibiting a large enhancement in the magnetic energy barrier and blocking temperature. The above single-molecule magnet materials have potential application in magnetic storage. More details are discussed in the article by Zheng et al. on pages 131—138.