The first actinide borosulfate series was synthesized solvothermally in 20% free SO3 oleum. (UO2)2[B2O(SO3OH)2(SO4)3] is an unconventional borosulfate and crystalizes in monoclinic space group _P_21/_n_ (_Z _= 4 _a: _10.871(1),_ b: _11.376(1),_ c: _14.817(1) Å, _β: _92.363(1)°)…