The syntheses, structures and magnetic properties of the series of dimeric organolanthanide(III) amides [Cp2Ln{2-NH-4,6-Me2pm}]2 [Ln = Nd (1), Gd (2), Dy (3), Yb (4) and pm = pyrimidine], which are formed from the deprotonation of 2-amino-4,6-dimethylpyrimidine by the corresponding lanthanide tris-cyclopentadienide, are reported. The synthesis and structure of [{Cp2Yb(2-NH-4-MeO-6-MeOpm)(2)(mu3-O)(YbCp)] (5), formed in a similar deprotonation reaction but in the presence of adventitious water, is also reported.