Reactions involving MI2 where M = Mg, Ca, Sr, Ba or Zn and M′TpC* where M′ = Na or Tl and TpC* = tris[3-methoxy-1,1-dimethyl)pyrazolyl]hydroborate in tetrahydrofuran are described leading to the isolation and characterization of the complexes TpC*MgI, I, TpC*CaI, II, TpC*SrI, III, TpC*SrI(THF), IV, TpC*BaI, V, TpC*BaI(pz*H), VI, where pz*H = 3-(2-methoxyl-1,1-dimethyl)pyrazole, TpC*BaI·½toluene, VII and TpC*ZnI, VIII. The compounds I, II, IV, VI, VII and VIII have been characterized by single-crystal X-ray crystallography. Compounds I and II are isostructural and are salt-like containing κ6-TpM+ cations and I− anions. In all other structures, the iodide is bound to the metal and TpC* is κ6 bonded to the group 2 M(2+) ions. Reactions involving TpC*CaI, II, and sodium or lithium alkoxides or amides failed to yield the amide or alkoxide calcium TpC* derivative, though related reactions involving TpC*ZnI, VIII, and KOSiMe3 proceeded quantitatively to yield κ3TpC*ZnOSiMe3, IX, which was also structurally characterized and shown to have the κ3-TpC* bound ligand.