A uniform array of one-dimensional molecular iodine wires is fabricated by introducing iodine molecules into the channels of AFI zeolite crystals through the vapor phase. The only possible wire structures are formed by linking individual iodine molecules along intramolecular bond axis into a single line. Polarization dependence of Raman intensity at modes of iodine species indicates that the wires are aligned perfectly along the c axis of AFI crystal. Polarized optical absorption as well as resonant Raman scattering reveal two wire species inside the channels of AFI zeolite: In- and (I2) n wires. © 2006 American Institute of Physics.