Abstract: Technetium-contaminated nickel is decontaminated by electrolytically dissolving nickel having a gross beta activity of at least about 74 Bq in a sulfuric acid solution having a pH between about 0.5 and 2.0. The applied voltage is from 2.0 v/cell to 5.0 v/cell for dissolving the nickel and contaminants while cathodically producing hydrogen gas. Technetium (+4) species in the acid solution is oxidized to the technetium (+7) species. The pH of the technetium-containing acid solution is adjusted to between 2.5 to 4.5. Particulates in the acid solution are filtered from the solution for reducing the gross beta activity of the acid solution to less than about 50 Bq/gm. Radioactive ions (including technetium complexes) are sorbed in an anionic exchanger and a cationic exchanger for reducing the gross beta activity of the acid solution to less than about 20 Bq/gm. After verifying the gross beta activity of the acid solution, the acid solution is either recycled or charged to a electrowinning step.