We report a comparative study of the quantal and classical treatments of single-electron charge transfer from the L and K shells of Li(ls22s) in collisions with He2+ ions at intermediate energies. Quantal calculations have been performed using coupledstate atomic orbital expansions with up to 43 pseudostates in the basis, within the impact parameter formalism, for impact energies of 8 to 2000 keV lab. Classical trajectory Monte Carlo calculations for L-shell capture, using a model potential for the active electron, have been performed for impact energies from 50 to 400 keV, and using an effective-charge model for K-shell capture at impact energies from 600 to 2000 keV lab. The quantal results are in close agreement with experiment over the whole energy range for the total capture cross section. The classical results give a good account of the shape of the cross section curve and are everywhere within *30% of the quantal values. A simple binning model applied to the classical results yields cross sections for capture into final n states which are in agreement with the quantal ones to the same accuracy.