The crystal and molecular structure of the polymethine dye 1,3-bis(dimethylamino)trimethinium perchlorate has been determined by X-ray diffraction techniques and refined to a residual of 6-9 %. The space group is Cc and the unit-cell parameters are a = 7.86 + 0.04, b = 18"93 + 0.12, e = 7.70_+ 0.05 A, fl=103"55+0.18 °. From the refined coordinates, the transition moments of the two non-parallel molecules in the unit cell were found to have direction cosines of 0.431, 0.879, 0.205 and 0.431, -0.879, 0.205 relative to orthogonal axes parallel to a*, b and e. The orientation of the dye molecules in the crystal is compared with predictions made by P. Gramaccioni and W. T. Simpson (unpublished results) on the basis of spectroscopic measurements, and the agreement between the X-ray and the optical studies is found to be excellent.