In this article, two optically-controlled spin transfer effects are proposed for pi-conjugated polymers. When such a polymeric molecule undergoes two-photon excitation, the charge of a spin carrier can be reversed, and simultaneously an applied external electric field drives the charge-reversed spin carrier to move in the opposite direction. As for a spinless carrier, the photoexcitation dissociates it into two spin carriers, forming entanglement. The coupling between the newly produced spin carriers and a ferromagnet will change the magnetoresistance. Both the fissions of spinless and spin carriers are ultrafast dynamical processes. By combining an electric field, magnetic field, and photoexcitation, two generic optically-control led ultrafast response organic spin valves are designed.