The mechanism of charge transport (CT) in a 1D atomistic model of an organic semiconductor is investigated using surface hopping nonadiabatic molecular dynamics. The simulations benefit from a newly implemented state tracking algorithm that accounts for trivial surface crossings and from a projection algorithm that removes decoherence correction-induced artificial long-range charge transfer. The CT mechanism changes from slow hopping of a fully localized charge to fast diffusion of a polaron delocalized over several molecules as electronic coupling between the molecules exceeds the critical threshold V ≥ λ/2 (λ is the reorganization energy). With increasing temperature, the polaron becomes more localized and the mobility exhibits a "band-like" power law decay due to increased site energy and electronic coupling fluctuations (local and nonlocal electron-phonon coupling). Thus, reducing both types of electron-phonon coupling while retaining high mean electronic couplings should be part of the strategy toward discovery of new organics with high room-temperature mobilities.