This paper proposes a predictive zero-voltage-switching (ZVS) control with improved ZVS time margin and limited variable switching frequency range for a 99% efficient megahertz (MHz) GaN totem-pole power-factor-correction (PFC) rectifier. The conventional ZVS control methods for totem-pole PFC may lead to zero ZVS time margin and ultra-wide switching frequency range. This paper proposes that the synchronous rectifier (SR) turn- off current is a new degree of freedom for the ZVS control. Thus, the proposed cycle-by-cycle predictive ZVS control method controls the SR turn- off currents to extend the ZVS time margin and to reduce the maximum switching frequency. With the proposed ZVS control, the minimum ZVS time margin and a limited maximum switching frequency can be realized in a MHz GaN-based totem-pole PFC. With the improved ZVS time margin, the reliability for realizing ZVS is significantly improved. With the limited maximum frequency and the limited frequency range, the difficulty in high-speed current sensing and digital control is reduced, and the frequency-related loss is also reduced, which is important for improving the light-load efficiency. To accurately extract the current and timing parameters for the proposed ZVS control, an analytical model for the ZVS totem-pole PFC is proposed. The proposed ZVS control and analytical model are applicable over the full input and output voltage range, and over the full load range. In addition, a hybrid current control is proposed and implemented based on the proposed ZVS control. Finally, a 3.2-kW MHz GaN totem-pole PFC prototype is developed and tested with full-range ZVS, minimum ZVS time margin, limited switching frequency range, 99% peak efficiency, and 130-W/in3 power density based on the proposed ZVS control and system control strategy. The realized efficiency, power level, and power density are among the best ever reported for the GaN-based totem-pole PFC.