The first example of an activated In-P-In-Cl-ring-containing compound, (Me3SiCH2)2 activated InP(SiMe3)2In-(CH2SiMe3)2Cl (1), was prepared by the reaction of (Me3SiCH2)2InCl and (Me3Si)3P in a 2:1 mole ratio. Similarly, the dimer containing an activated In-P-In-P core, [(Me3SiCH2)2InP(SiMe3)2]2 (2), was prepared by reaction in a 1:1 mole ratio. X-ray crystallographic analyses showed the activated In-P-In-Cl ring of 1 to be nonplanar while the activated In-P-In-P ring of 2 is planar. Compound 1 belongs to the triclinic system, space group P1BAR (C(i)1), with two molecules in a unit cell of dimensions a = 12.581 (1) angstrom, b = 19.470 (2) angstrom, c = 9.643 (1) angstrom, alpha = 89.75 (1)-degrees, beta = 112.91 (1)-degrees, and gamma = 100.68 (1)-degrees. Compound 2 crystallizes in the orthorhombic system, space group Pbcn (D2h14), with four molecules in a unit cell of dimensions a = 12.782 (2) angstrom, b = 21.482 (3) angstrom, and c = 18.651 (3) angstrom. Compound 2 reacts with 2 equiv of (Me3SiCH2)2InCl to yield 1 as a major product, as evidenced by H-1 and C-13{H-1} NMR and melting point data.