We investigate pulse design problems arising in diverse applications in quantum science and technology. In modern approaches, pulse design is cast as an ensemble control problem involving the control of a continuum of nuclear spin systems, which, however, is typically challenging to solve. In this paper, we present a new pulse design paradigm by introducing moment representations of the spin ensemble system and transforming the ensemble control problem associated to pulse design to a moment control problem. We show that feasible and optimal pulses can be effectively designed using the moment system with performance guarantees across the entire ensemble. We also illustrate the versatility and robustness of our moment-based approach by designing uniform and selective pulses essential to enable prominent applications in magnetic resonance.