Single-electron charge transfer between He2+ and NH3 and H2S was investigated at the projectile energy of 70 eV by the translational energy spectroscopy method with a resolution of 120 meV. The products were He+*(P-2) and the ground state molecular ion. Populations of the vibrational states of the molecular ion were derived from the spectra. The vibrational state distributions differ only slightly from the. distributions obtained by photoelectron spectroscopy and the differences can be qualitatively accounted for by distortions of the equilibrium configuration of the target molecule by the Physics.