To determine the possibility of technological use of coherent Bremsstrahlung beams the photonuclear transmutation doping of silicon by aluminum upon γ-quantum irradiation from the aligned single-crystal target was studied. An increase in aluminum concentration by approximately ten times was obtained upon γ-radiation of silicon from the crystalline target aligned by the crystallographic axis 〈111〉 along the direction of the electron beam with the energy of 1200 MeV. The orientation effect of an increase in the yield of γ-radiation from silicon and tungsten crystals in the range of energies of accelerated electrons of 300–1200 MeV was examined. This result is essential for the estimation of a possible minimum energy of electrons at which the use of the orientation effect is reasonable.