Dispersion laws and states (i.e. probability of finding) of Frankel excitons in ultra-thin molecular films are found using a well-known method of Green’s functions. Space boundaries and changes of energetic parameters on boundaries are considered as perturbations. The cubic crystalline system with complex cell consisted of two molecules (a and b), i.e. bimolecular film, was analyzed in harmonic approximation, and then compared with the results obtained for simple cubic cell systems (i.e. monomolecular film). In both cases the energy spectra show sharp discrete levels, although the energy spectra of bimolecular films split into two zones with discrete levels. Probability of finding exciton in the mono- or bimolecular ultra-thin films is significantly influenced by the perturbation and the values of on-site energies of molecules a and b. Obtained conditions of the existence of localized exciton states at boundaries are of special interest.