Infrared and Raman spectral properties of the organic composites obtained by direct solid-solid charge-transfer (CT) reaction between bis(ethylenedioxy)tetrathiafulvalene (BEDO-TTF) and iodine are investigated for the first time. The band attribution, an evaluation of the average charge on the donor molecule, changes of the BEDO-TTF spectra after composite formation and an analysis of the plasma-edge-like dispersion are presented and discussed.