Treatment of [Cp*(2)U(NCMe)(5)]X(2) [Cp* = C(5)Me(5), X = BPh(4) (1) or I (1')] or Cp*(2)UI(2) in acetonitrile with the polydentate aromatic nitrogen bases phen, terpy and R(4)btbp led to the formation of the linear uranium metallocenes [Cp*(2)U(NCMe)(3)(phen)]X(2) [X = BPh(4) (2), I (2')], [Cp*(2)U(NCMe)(2)(terpy)][BPh(4)](2) (4), [Cp*(2)U(NCMe)(Me(4)btbp)][BPh(4)](2) (5) and [Cp*(2)U(NCMe)(CyMe(4)btbp)][X](2), [X = BPh(4) (6), I (6')], [phen = 1,10-phenanthroline, terpy = 2,2':6,2''-terpyridine, Me(4)btbp = 6,6'-bis-(3,3,6,6-tetramethyl-1,2,4-triazin-3-yl)-2,2'-bipyridine, CyMe(4)btbp = 6,6'-bis-(3,3,6,6-tetramethyl-cyclohexane-1,2,4-triazin-3-yl)-2,2'-bipyridine]. The bent metallocene [Cp*(2)U(phen)(2)][BPh(4)](2) (3) was isolated from the reaction of 1 and two molar equivalents of phen in THF. The X-ray crystal structures of 2.2MeCN, 3.2THF, and 6'.2MeCN were determined.