Two thallium scorpionate complexes: dihydrobis (3-phenyl-4-cyanopyrazolyl) boratothallium(I) (TlBp Ph,4CN), C 20H 14BN 6Tl and dihydrobis(3-tert-butyl-4-cyanopyrazolyl) boratothallium(I) (TlBp t-Bu,4CN), C 16H 22BN 6Tl have been prepared and characterized by X-ray diffraction. Both compounds crystallize in monoclinic space groups, TlBp Ph,4CN in P2 1/n with a = 4.2039(3) Å, b = 26.2211(17) Å, c = 16.611(1) Å, β = 90.199(3)°, and TlBp t-Bu,4CN in P2 1/c with a = 13.8578(5) Å, b = 9.6741(4) Å, c = 14.2790(5) Å, β 95.141(2)°. The two complexes show similar structures with elongated metal-ligand bonds and intermolecular interactions between the metal ion and cyano substituents, allowing the potential construction of cyanobridged coordination polymers.