The combination of magnetic interaction with high magnetic anisotropy provides a promising way for modulating/fine-tuning molecular magnetic behaviors. Here, we show the building block approach for the synthesis of a family of dilanthanide single-molecule magnets (SMMs) bridged with a cyanometallate starting from a monolanthanide SMM. Contingent on the central para-/diamagnetic [M(CN)(6)](3-) (M = Fe, Co) integrated between two highly anisotropic pentagonal-bipyramid Dy(III) subunits, the remanence of magnetization is OFF/ON below 15 K and they respectively display a record reversal barrier of 659 K among d-f SMMs and 975 K among cyanobridged SMMs.