Crystal frameworks that can accommodate a wide range of elements, oxidation states, and stoichiometries are an important component of solid-state chemistry. These frameworks allow for unique comparisons of different metal-cation compositions with identical atomic arrangements. The mineral Lyonsite, alpha-Cu3Fe4(VO4)(6), is emerging as the archetypal framework structure for a large class of materials, similar to known frameworks such as perovskite, garnet, apatite, and spinel. The new lyonsite-type oxides Li2.82Hf0.795Mo3O12 and Li3.35Ta0.53Mo3O12, in which hafnium and tantalum retain their highest oxidation states, are presented to advance the concept of the lyonsite structure as an adaptable framework.