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In the past two decades, tremendous progress has been made in the field of single-molecule magnets (SMMs), which not only achieves breakthroughs in various key indicators (flipping energy barrier and hysteresis temperature), but also expands SMMs of various types (3d, 4f, 3d–4f and 5f) and different connection methods. Among the many different types of SMM mentioned above, the SMM based on the 4f metal center has made the biggest breakthrough. Introducing 3d metal ions into lanthanide complexes to form 3d–4f heterometallic complexes can promote strong magnetic exchange between multiple metal centers, resulting in magnetic properties different from 3d and 4f complexes. Therefore, the expansion of the structure and magnetic properties of 3d–4f heterometallic complexes can promote the progress in the field of SMM. In this review, we summarize the structure and magnetic properties of 3d–4f heterometallic complexes formed by different types of organic ligands. [ABSTRACT FROM AUTHOR]