A series of mono- and binuclear Lewis acid-base complexes of the formulas N[CHCHN(Pr)]P→LA [LA = BH (8), Ga(CF) (10), GaCl (11)], LA←N[CHCHN(Pr)]P [LA = Al(CF) (6a), AlMe (6b), AlEt (6c), AlBu (6d), BF (13)], and LA←N[CHCHN(Pr)]P→LA [Lewis acid (LA) = Al(CF) (7a), AlMe (7b), AlEt (7c), AlBu (7d), AlCl (7e), BH (9)] were generated from reactions of Verkade's base, N[CHCHN(Pr)]P (1), with various boron-, aluminum-, and gallium-containing Lewis acids, and characterized by multinuclear NMR spectroscopy. {N[CHCHN(Pr)]P→CH}[BF] (5) was synthesized via the treatment of 1 with [CH][BF]. The reaction of 1 with B(CF), followed by the addition of [PhC][BCl], gave rise to the rearranged borate salt [PNCH(Pr)][BCl] (3), while treating 1 with [PhC][BCl] exclusively afforded {N[CHCHN(Pr)]PH}[BCl] (4). Reactions of 1 with 2 equiv of GaCl and BF, respectively, afforded the novel phosphenium gallate and borate salts 12a, 12b, and 15. The solid-state structures of 1, 3-5, 6b, 7a, 7b, 7e, 8, 10, 11, 12b, 13, and 15 were determined by X-ray crystallography.