Quantum-dynamical simulations are used to investigate the interplay of exciton delocalization and vibronically induced internal conversion processes in the elementary charge separation steps at regioregular donor-acceptor heterojunctions. Ultrafast internal conversion leads to efficient deexcitation within the excitonic and charge transfer manifolds, thus modifying the charge separation dynamics. We address a model donor-acceptor junction representative of regioregular P3HT-PCBM, using high-dimensional quantum dynamics simulations by multiconfigurational methods. While partial trapping into an interfacial charge separated state occurs, long-range charge-separated states are accessed as previously demonstrated in the work of Tamura and Burghardt [J. Am. Chem. Soc. 2013, 135, 16364]. For an H-aggregate type, stacked donor species, the initial bright state undergoes ultrafast internal conversion within the excitonic manifold, creating multiple charge transfer pathways before reaching the lowest-energy dark exciton, which is uncoupled from the charge transfer manifold. This process profoundly affects the charge separation mechanism and efficiency. For small energetic offsets between the interfacial excitonic and charge transfer states, a delocalized initial bright state proves less prone to electron-hole capture by the interfacial trap than a localized, vibronic wavepacket close to the interface. For both delocalized and localized initial states, a comparable yield of free carriers is obtained, which is found to be optimal for energetic offsets of the order of the Coulomb barrier to charge separation. Interfacial trapping is significantly reduced as the barrier height decreases with fullerene aggregation. Despite the high-dimensional nature of the system, charge separation is an ultrafast coherent quantum process exhibiting oscillatory features as observed in recent experiments.