We describe a method for improving coherent control through the use of detailed knowledge of the system's Hamiltonian. Precise unitary transformations were obtained by strongly modulating the system's dynamics to average out unwanted evolution. With the aid of numerical search methods, pulsed irradiation schemes are obtained that perform accurate, arbitrary, selective gates on multiqubit systems. Compared to low power selective pulses, which cannot average out all unwanted evolution, these pulses are substantially shorter in time, thereby reducing the effects of relaxation. Liquid-state nuclear magnetic resonance techniques on homonuclear spin systems are used to demonstrate the accuracy of these gates both in simulation and experiment. Simulations of the coherent evolution of a three-qubit system show that the control sequences faithfully implement the unitary operations, typically yielding gate fidelities on the order of 0.999 and, for some sequences, up to 0.9997. The experimentally determined density matrices resulting from the application of different control sequences on a three-spin system have overlaps of up to 0.99 with the expected states, confirming the quality of the experimental implementation.