M(TpyNO2)(NO3)3(H2O)·THF (M = La, Nd, Sm, Eu, Tb, Am; TpyNO2 = 4'-nitrophenyl terpyridyl) have been prepared from the reaction of M(NO3)3· nH2O with TpyNO2 in THF. Structural analysis shows that the metal centers are 10-coordinate, providing the first example of AmIII with this coordination number. Further spectroscopic and theoretical evaluation of these complexes reveals utilization of the 5f orbitals in bonding in the AmIII complex. Comparison of Nd-L, Eu-L, and Am-L bond distances demonstrates that some caution should be taken in comparing EuIII versus AmIII in extraction experiments.