The coprecipitation of transuranium elements and technetium from alkaline solutions and from simulants of Hanford Site tank wastes has been studied in reducing and oxidizing conditions on uranium(IV,vT) hydroxocompounds, tetraakylammonium perrhenate and perchlorate, and on hydroxides of Fe(m), Co(III), Mn(II), and C r o using the Method of Appearing Reagents (MAR). Coprecipitations in alkaline solution have been shown to give high decontamination factors (DF) at low content of carrier and in the presence of high salt concentrations.Uranium(IV) hydroxide in concentrations higher than 3~1 0 -~ M coprecipitates Pu and Cm in any oxidation state from 0.2 to 4 M NaOH with DFs of 110 to lo00 and Np and Tc with DFs of 51 to 176. UraniumCvI), introduced as a sodium uranate precipitate or the soluble peroxocomplex salt NaUO2(02)3, can be partially reduced in 0.2 to 2 M NaOH by hydrazine to U30~.nH20 in the presence of (1 to 5 )~1 0 -~ M Tc(VII). The Tc(VlI) is first reduced to Tc(IV). The product U308.nH20, at 0.012 to 0.05 M uranium, coprecipitates Np, Pu, Cm, and Tc in any oxidation state with DFs greater than 100 from 0.2 to 1.5 M NaOH. Increasing alkali concentration to 4 M NaOH decreases the DFs slightly for TRU and drastically for Tc. Coprecipitation under the same conditions from simulated tank waste containing 3.2 M NaOH, 0.04 M C1-05-and 11 complex-forming salts yields the following DFs: Np-12, Pu-27, Cm-35, Tc-3. The decrease of DFs in the waste simulant is associated with complex formation and with inhibition of Np and Tc coprecipitation by the Cr(m) hydroxide that is formed before Np(IV) and Tc(IV). Coprecipitated Tc may be effectively leached from U30p-nH20 by oxidation of Tc(IV) to Tc(VII) by use of dilute H202 or by NaOH solution and air bubbling. Under these same conditions, more than 99% of the Pu is retained in the solid phase. iii