This Minireview covers the design and characterization of coordination lanthanide complexes involving TTF-based ligands. The specific design of TTF-based ligands allowed the isolation of complexes with magnetic properties such as Single-Molecule Magnets (SMMs) behavior and the studies of magnetic modulations due to supramolecular interaction, molecular engineering, magnetic dilution as well as isotopic enrichment. A careful design leads to TTF-based ligands displaying several coordination sites in order to rationally elaborate polynuclear systems with multi-SMM behavior or to auto-assembly SMMs. Their redox activity allowed the investigation of coordination lanthanide complexes in several oxidation states and their consequences on optical and magnetic properties. The complete experimental and theoretical studies of such systems contributed to the understanding of the magnetic properties of lanthanide ions for futures applications in high density storage and quantum computing.