Abstract Click to copy section linkSection link copied! Reaction of Cp*UI2(THF)3 (Cp* = pentamethylcyclopentadienide; THF = tetrahydrofuran) with NaR3TerNH (R3Ter = 2,6(2,4,6-R3C6H2)2C6H3; R = Me, Et, iPr) gave the U(III) monoiodide complexes Cp*(R3TerNH)UI (R = Me, 1-Me; R = Et, 2-Et; R = iPr, 3-iPr). These complexes contain a functionalizable iodide position which reacts favorably with NaBH4 to give the κ3-borohydride complexes Cp*(R3TerNH)U(H3BH) (R = Me, 4-Me; R = Et, 5-Et; R = iPr, 6-iPr).