Abstract Uranium and thorium tetrachloride (UCl 4 and ThCl 4) were obtained via the ammonium chloride route from UH 3 and thorium metal respectively, with the ternary chlorides (NH 4) 2 UCl 6 and (NH 4) 2 ThCl 6 acting as intermediates. The crystal structure of UCl 4 was refined (R= 0.031, R w= 0.026). Cs 2 UCl 6 and Cs 2 ThCl 6 were synthesized, their lattice constants refined from powder data, and the crystal structure of Cs 2 UCl 6 ...