Four crystal structures of the title complexes have been analyzed by X-ray crystallography. 1 : C80H68N17Nd, a = 17.0545(6) Angstrom, c = 22.807(3) Angstrom, tetragonal, P4/ncc, Z = 4. 2 : C80H68N17Gd, a = 17.399(8) Angstrom, c = 11.377(6) Angstrom, tetragonal, P42(1)2, Z = 2. 3 : C80H70N17OHo, a = 18.096(5) Angstrom, c = 11.079(6) Angstrom, tetragonal, P42(1)2, Z = 4. 4 : C80H70N17OLu, a = 18.171(3) Angstrom, c = 10.987(4) Angstrom, tetragonal, P4/nmm, Z = 2. The [Ln(III)Pc(2)](-) and [NBu(4)(n)](+) ions in each crystal stack alternately in a column along the 4-fold axis. The Ln(III) cation of each [Ln(III)Pc(2)](-) is eight-coordinated by two phthalocyanato dianions (Pc). The interplanar distances between the two Pc rings have a linear relationship to the ionic radii of the central Ln(III) cations. The skew angles between the two Pc rings are 6.2, 34.4, 43.2, and 45.0 degrees for the Nd, Gd, Ho, and Lu complexes, respectively. The skew angle seems to depend on the strength of the pi-pi interaction between the two Pc rings.