We demonstrated our synthetic strategy's application in different combinations of Ln 3+ , opening the possibility of a systematic study of the interactivity and cooperativity between Ln, as well as intentional design for applications in magneto-optics and quantum information science. Furthermore, the synthetic methodology we have described should be applicable to a wide range of both metal ions and asymmetric bridging ligands. This provides the opportunity to access new multimetallic systems featuring ionic and non-directionally bonding metals such as those in the f-and s-blocks and will allow the chemistry of such metals to be explored in new environments.