Modulating Magnetic Performance in Dyiii Single Ion Magnets with N5o2 Ligands

[Dy (LMe)(H<inf>2</inf>O)]CF<inf>3</inf>SO<inf>3</inf>·0.25H<inf>2</inf>O (1·0.25H<inf>2</inf>O), where H<inf>2</inf>LMe is the reported ligand 2,2′-(((pyridine-2,6-diylbis (methylene))bis((pyridin-2-ylmethyl)azanediyl))bis (methylene))bis(4-methylphenol), shows the DyIII ion in an N<inf>5</inf>O<inf>3</inf> environment, with triangular dodecahedral geometry (D<inf>2d</inf> symmetry). 1·0.25H<inf>2</inf>O is a single ion magnet (SIM) with an energy barrier for spin reversal of 510 K, and open hysteresis loops up to 8 K. The magnetostructural comparison of 1·0.25H<inf>2</inf>O with some closely related complexes and with other eight-coordinated SIMs with high energy barriers (> 300 K) allows to draw some conclusions to enhance the magnetic performance in these nanomagnets with non-purely axial geometries. Ab initio calculations complement and support the experimental results. © 2024 The Author(s). Applied Organometallic Chemistry published by John Wiley & Sons Ltd.