Abstract: In this review, we present the recent use of anilato-based ligands (derivatives of the 3,6-disubstituted-2,5-dihydroxy-1,4-benzoquinone dianion = C₆O₄X₂²⁻) to build heterometallic 2D magnets. Among the different metal couples, the Mn(II)Cr(III)-containing layers are, by far, the most studied and characterized ones. We will show the structures and properties of the extended families of layered magnets formulated as A[M^IIM^III(C₆O₄X₂)₃]·G and A₂[M^IM^III(C₆O₄X₂)₃]·G (A = monocation; X = Cl, Br, CN,··· G = solvent molecules). We also focus on how it is possible to modulate the magnetic properties of these magnets (ordering temperatures and coercive fields) by simply changing the cation, the X groups, the solvent molecules and the oxidation state of the anilato ligand. Moreover, the tune of the magnetic properties of these layered magnets in a post-synthetic way is also shown.

Key words: layered magnets, anilato ligands, heterometallic compounds, magnetic properties, molecule-based magnets