Using the existing architecture of [Dy(Tp2-py)F]+ that supports a terminal Dy-F bond, the synthesis and isolation of [Dy(Tp2-py)F(THF)2](PF6) and its diamagnetic yttrium analogue have been achieved. Alternating current magnetic susceptibility studies show an increased effective energy barrier of Ueff = 661(6) cm-1 (951(8) K), the highest yet reported for a high coordinate (n > 8) lanthanide single-ion magnet.