<p><a></a><a></a><a><b>Three six-coordinate Dy(III) single-molecule magnets (SMMs) [Dy(O<sup>t</sup>Bu)<sub>2</sub>(L)<sub>4</sub>]<sup>+</sup> with <i>D</i><sub>4h</sub> local symmetry are obtained by optimising the equatorial ligands. Compound 1 where L = 4-phenylpyridine shows an energy barrier (<i>U</i><sub>eff</sub>) of 2075(11) K, which is the third largest <i>U</i><sub>eff</sub>, and the first <i>U</i><sub>eff</sub> > 2000 K for SMMs with axial-type symmetry so far.</b></a></p>