The molecular orientation and relaxation behavior was studied by rheooptical FTIR spectroscopy during the uniaxial deformation of epoxy resins prepared from the diglycidyl ether of butanediol and novolacs on the basis of bisphenol A. The investigation of orientation phenomena was performed in both the rubbery and the glassy state of the epoxies. Results are discussed with regard to the respective mechanism of deformation. Moreover, the effect of temperature, strain rate, and the molecular weight of the novolacs used on the orientation behavior and the mechanical properties was studied. A significant influence of these, parameters on the molecular deformation behavior was observed. The reversibility of the orientation at temperatures above and below the glass transition temperature was examined. Epoxy films were subjected to successive loading-unloading cycles including elongation, relaxation, and annealing. The investigations show that the orientation is completely reversible in the rubbery state, but it is only partly reversible below the glass temperature.