The synergistic co-production of ceramic fibers from fly ash and coal gangue offers a promising path for their high-value utilization. However, research in this area remains limited, hindering its broader application. This study employs numerical simulations to assess the influence of high-wheel rotational speed and melt temperature on the mass of inter-wheel melt transfer, as well as their effects on ligament size and slag-ball fraction. The results show that the high wheel, responsible for melt pre-fragmentation and transfer, plays a crucial role in determining the mass of inter-wheel melt transfer and controlling ligament dimensions. In contrast, the low wheel does not directly affect ligament size but aids in transforming pre-fragmented droplets into ligaments and modulates their dispersion. Melt temperature impacts both transfer mass and ligament size by modifying melt properties. The slag-ball fraction increases with the melt temperature and decreases with the high-wheel speed, while the low-wheel speed has a negligible effect. Under the optimal operating conditions of a melt temperature of 1745 °C and equal rotational speeds of 10,000 rpm for both the high and low wheels, a ligament structure with a relatively concentrated size distribution is obtained, with the slag-ball fraction effectively controlled within the range of 8–13%.