<p>Carbon fiber–reinforced plastic (CFRP)/Ti6Al4V stacks are widely used in the aircraft industry to increase structural strength, reduce overall weight, and lower life cycle costs. A high drilling temperature has always been an unavoidable issue in stack drilling, resulting in severe delamination of CFRPs, the formation of large Ti6Al4V burrs, and poor hole surface quality. Therefore, accurately predicting the drilling temperature is crucial when drilling CFRP/Ti6Al4V stacks. However, differences in the thermal properties of the two materials and their heat transfer at the interface present challenges. This study proposes a novel temperature predictive model for low-frequency vibration-assisted drilling (LFVAD) of CFRP/Ti6Al4V stacks. The influences of heat transfer at the CFRP/Ti6Al4V interface and separation motion in LFVAD are considered in the model to predict the stack drilling temperature distribution, and the heat partition ratios of the two materials are also calculated. Internal air cooling, minimal quantity lubrication (MQL), and supercritical carbon dioxide (ScCO₂) cooling strategies are applied in the drilling experiments to verify the accuracy of the proposed model and to study the influence of the drilling temperature on the hole quality. The results show that the prediction errors of the temperature in the CFRP and Ti6Al4V picked regions during LFVAD under the internal air cooling strategy are within 6.2% and 8.9%, respectively. By significantly reducing the heat flowing into the workpiece, the ScCO₂ cooling strategy can effectively reduce the drilling temperature of the CFRP, interface, and Ti6Al4V by 15%, 72%, and 33%, respectively, compared with the internal air cooling strategy. Moreover, MQL reduces the drilling temperature of Ti6Al4V by 27%. This research contributes to a deeper understanding of the heat transfer mechanisms in LFVAD of CFRP/Ti6Al4V stacks and provides guidance for improving drilling quality.</p>