The metathetical reaction of 2-(dimethylamino)benzyllithium (Bz(N)Li) with GaCl3 afforded the salt [Bz(2)(N)Ga]-[GaCl4] (4), the X-ray crystal structure of which revealed a four-coordinate cationic gallium center featuring two Ga-C sigma-bonds and two N-->Ga dative bonds. (Crystal data for 4 : monoclinic, space group P2(1)/n, a = 11.519(2) Angstrom, b = 18.254(4) Angstrom, c = 12.506(3) Angstrom, beta = 117.40(3)degrees, V = 2334.6(9) Angstrom(3), Z = 4, R = 0.545). Two Ga ... Cl interionic contacts, while somewhat long, are sufficiently strong to render the geometry of 4(+) roughly midway between tetrahedral and octahedral. Treatment of 1,4-di-tert-butyl-1,4-diazabutadiene (DAB) with 2 equiv of GaCl3 afforded [(DAB)GaCl2][GaCl4] (7), which, by means of X-ray analysis, was shown to possess a cation (7(+)) with localized C=N bonds and N-->Ga dative interactions with a [GaCl2](+) moiety. (Crystal data for 7 : orthorhombic, space group Pbca, a = 11.882(2) Angstrom, b = 17.289(3) Angstrom, c = 20.424(4) Angstrom, V = 4195.5(11) Angstrom(3), Z = 8, R = 0.460). The structure of 7(+) is relevant to discussions of the bonding in both neutral DAB complexes of the group 13 elements and the skeletally isoelectronic anion [Me(4)C(4)GaCl(2)](-) (9(-)). The structure of the [NEt(4)](+) salt of the latter (9) has been determined by X-ray diffraction. (Crystal data for 9 : monoclinic, space group P2(1)/n, a = 9.967(1) Angstrom, b = 13.073(2) Angstrom, c = 15.345(2) Angstrom, beta = 96.76(1)degrees, V = 1985.5(4) Angstrom(3), Z = 4, R = 0.721).