θ-(BETS) 4 [Fe(CN) 5 NO] (1), (BETS) 2 [RuBr 5 NO] (2), and (BETS) 2 [RuCl 5 NO] (3) [BETS = bis(ethylenedithio)tetraselenafulvalene] have been prepared by electrocrystallisation of BETS using [Fe(CN) 5 NO] 2− or [RuX 5 NO] 2− , X = Cl or Br, as supporting electrolytes and 1,1,2-TCE/ethanol (10 vol%) for 1, nitrobenzene/1,2-DCE (40 vol%)/ethanol (10 vol%) for 2, and benzonitrile/ethanol (10%) solutions for 3 as solvents.Compound 1 exhibits a metallic behaviour down to 40 K, 2 behaves as a semiconductor and 3 as an insulator. The crystal