An organoindium compound with an In-Se bond, [(Me3CCH2)2InSePh]2, has been synthesized and characterized by elemental analyses, IR, H-1 NMR, and C-13 NMR spectroscopy, cryoscopic molecular weight studies, and an X-ray structural study. The dimeric molecule crystallizes in the centrosymmetric monoclinic spacegroup P2(1)/c (No. 14) with a = 18.973 (4) angstrom, b = 10.105 (1) angstrom, c = 19.998 (6) angstrom, beta = 103.66 (2)-degrees, V = 3725.4 (14) angstrom3, and Z = 4. Diffraction data (Mo K-alpha, 2-theta = 5-45-degrees) were collected on a Siemens R3m/V automated four-circle diffractometer, and the structure was solved and refined to R = 3.44% and R(w) = 3.73% for those 2557 unique data with \F(o)\ > 6-sigma(\F(o)\) (R = 8.35% for al 4891 data). The four-membered ln2Se2 ring has a butterfly arrangement with the phenyl groups in the anti position relative to the ring. The In-C(neopentyl) distances range from 2.135 (11) to 2.168 (10) angstrom, while In-Se bond distances range from 2.748 (1) to 2.756 (1) angstrom. There is some rotational disorder of the methyl groups within (at least) one of the methyl (-CH2CMe3) groups.