A series of pseudosymmetrical structures of formula K-10(M2OnF11-n)3(X) (M = V and Nb, n = 2, X = (F2Cl)(1/3), Br, Br-4/2,I-4/2; M = Mo, n = 4, X = Cl, Br-4/2, I-4/2) illustrates generation of polar structures with the use of Lambda-shaped basic building units (BBUs). For a compound to belong to a polar space group, dipole moments of individual species must be partially aligned. Incorporation of d(0) early transition metal polyhedral BBUs into structures is a common method to create polar structures, owing to the second-order Jahn-Teller distortion these polyhedra contain. Less attention has been spent examining how to align the polar moments of BBUs. To address alignment, we present a study on previously reported bimetallic BBUs and synthesized compounds K-10(M2OnF11-n)(3)X. These materials differ in their (non)centrosymmetry despite chemical and structural similarities. The vanadium compounds are centrosymmetric (space groups P (3) over bar m1 or C2/m) while the niobium and molybdenum heterotypes are noncentrosymmetric (Pmn2(1)). The difference in symmetry occurs owing to the presence of linear, bimetallic BBUs or Lambda-shaped bimetallic BBUs and related packing effects. These Lambda-shaped BBUs form as a consequence of the coordination environment around the bridging anion of the metal oxide fluoride BBUs.