A new composite material composed of GaSe and CdSe has been obtained by treatment of GaSe single-crystal lamellas in Cd vapors at temperatures of 773853 K and intercalation of Cd interlayers. The structure and optical properties of the GaSe-CdSe composite material have been studied. The content of CdSe crystallites was found to grow with increasing treatment temperature or with increasing duration of treatment at a constant temperature. Analysis of XRD, PL, XPS, AFM, and Raman patterns has shown that the heterogeneous composite composed of micro and nanocrystallites of CdSe in GaSe can be obtained by Cd intercalation in a temperature range of 753853 K. On the basis of Raman spectrum, the vibrational modes of the composite have been identified. The PL of these materials contains emission bands of free and bound excitons, donor-acceptor bands, and bands of recombination via impurity levels. The PL emission spectra measured at a temperature of 78 and 300 K for the composites result from the overlapping of the emission bands of the components of GaSe doped with Cd and the CdSe crystallites.