Centrifugal atomization is a rapid solidification technique for producing metal powders. However, its wide application has been limited to the production of common metal powders and their corresponding alloys. Therefore, there is a lack of research on the production of novel materials such as metallic glasses using this technology. In this paper, aluminum-based glassy powders (Al86Ni8Y4.5La1.5) were produced by centrifugal atomization. The effects of disk speed, atomization gas, and particle size on the cooling rate and the final microstructure of the resulting powder were investigated. The powders were characterized using SEM and XRD, and the amorphous fractions of the atomized powder samples were quantified through DSC analysis. A theoretical model was developed to evaluate the thermal evolution of the atomized droplets and to calculate their cooling rate. The average cooling rate experienced by the centrifugally atomized powder was calculated to be approximately 7 × 105 Ks−1 for particle sizes of 32.5 μm atomized at 40,000 rpm in a helium atmosphere. Amorphous fractions from 60% to 70% were obtained in particles with sizes of up to 125 μm in the most favorable atomization conditions.