We report on the synthesis of two dysprosium(III) containing complexes with double-decker and triple-decker sandwich structures. These two complexes have formulae (NMe4)[Dy(dsp)2] (1) and [Dy2(dsp)3(EtOH)] (2), where H2dsp is a salen type ligand. Both compounds were characterized by X-ray structural analysis, UV–Vis, IR spectral and magnetic studies. Complex 1 crystallized in the space group Pna21. This X-ray structural data provides the first example of the structure of [Ln(dsp)2]−. Compound 2 crystallized in a triclinic space group View the MathML source. In both cases, two similar but symmetry-independent molecules are present. The UV–Vis spectra of the complexes indicate that they are ligand-based π–π∗ transitions, which was further supported by DFT calculations. Both compounds display field-induced out-of-phase signals. In particular, step-wise slow magnetization relaxation processes are observed in the case of complex 2. This indicates that compound 1 and 2 undergo slow magnetization relaxation when a small dc magnetic field is applied.