Abstract Reaction of LaX3(THF)n (X = Cl, I) with two equiv. of K(TpMe2) gave good yields of the bis-Tp complexes [La(TpMe2)2X] (X = Cl (1); I (3)). However, the formation of 1 and 3 is always accompanied by significant amounts of La(TpMe2)2(κ2-pzMe2) ([pzMe2]− = 3,5-dimethyl-pyrazolato) (2). The pyrazolato complex 2, which presumably arises from decomposition of the [TpMe2]− moiety during salt metathesis, was independently prepared in good yield from 1 and in situ generated [pzMe2]−. The solid-state structures of 1 and 2 were determined by single-crystal X-ray diffraction studies. Subsequent reactions of halogeno-TpMe2 complexes 1 and 3 with various alkali metal salts MR (M = Li, R = CH2SiMe3, Ph, N(SiMe3)2; M = K, R = OAr) gave M(TpMe2) as the major product. Alternatively, the mono-Tp bis(aryloxide) derivatives [Ln(TpMe2)(OC6H2-2,6-tBu-4-Me)2] (Ln = La (4); Nd (5)) were obtained in high yields by salt metathesis of [Ln(OC6H2-2,6-tBu-4-Me)3] with one equiv. of K(TpMe2).