The ability to sense and control nuclear spins near solid-state defects might enable a range of quantum technologies. Dynamically decoupled radio-frequency (DDrf) control offers a high degree of design flexibility and long electron-spin coherence times. However, previous studies have considered simplified models and little is known about optimal gate design and fundamental limits. Here, we develop a generalized DDrf framework that has important implications for spin sensing and control. Our analytical model, which we corroborate by experiments on a single NV center in diamond, reveals the mechanisms that govern the selectivity of gates and their effective Rabi frequencies, and enables flexible detuned gate designs. We apply these insights to numerically show a 60× sensitivity enhancement for detecting weakly coupled spins and study the optimization of quantum gates in multiqubit registers. These results advance the understanding for a broad class of gates and provide a toolbox for application-specific design, enabling improved quantum control and sensing.