Reduction of (C6F5NHCH2CH2)(2)NMe with LiAlH4 produces (3,4,5-C6F5NHCH2CH2](2)NMe (H-2[F3NMe]) in good yield. Reactions between H2F3NMe] and MCl4 (M = Mo, W) in the presence of NEt3 yield pseudooctahedral paramagnetic compounds of the type [Et3NH]([F3NMe]MCl3). Treatment of [Et3NH]([F3NMe]MoCl3) with 3 equiv of Me3CCH2MgCl produced five-coordinate [F3NMe]Mo(CH2CMe3)(CCMe3), while treatment with 3 equiv of Me3SiCH2MgCl produced five-coordinate paramagnetic [F3NMe]Mo(CH2SiMe3)(2). Upon heating, F3NMe/Mo(CH2SiMe3)2 is converted into diamagnetic ([F3NMe]Mo(CSiMe3))(2). Reactions between [Et3NH]([F3NMe]WCl3) and Me3CCH2MgCl or Me3SiCH2MgCL lead to five-coordinate diamagnetic complexes of the type [F3NMe]W(CH2R)(CR), where R = CMe3, SiMe3 respectively. X-ray studies confirmed the structures of [F3NMe]Mo(CH2CMe3)(CCMe3) and ([F3NMe/Mo(CSiMe3))(2).