We present a theoretical investigation of the impulsive orientation that can be induced by exposing a sample of state-selected NO molecules to the combination of a dc field and a short laser pulse. A strong degree of laserfield-free alignment and orientation is already achievable at moderate intensities and can be further improved by tailoring the temporal profile of the laser pulse. The alignment and orientation are only limited by the maximum value of the applied dc field and the pulse energy in the femtosecond laser pulse. Using an evolutionary algorithm coupled to a non-perturbative calculation of the timedependent Schrödinger equation, the solutions that are obtained suggest that (cosθ) = 0.964 is experimentally achievable. © IOP Publishing Ltd and Deutsche Physikalische Gesellschaft.