A control scheme with high reliability and excellent tracking performance is essential for the automatic operation of high-speed trains (HSTs). In this study, a novel discrete-time data-driven predictive sliding mode control (DDPSMC) scheme is proposed for multi-power unit HSTs. Initially, a nonlinear integral terminal sliding mode surface was designed to replace the traditional linear sliding mode function, thereby achieving a rapid system error convergence and alleviating chattering. Then, receding horizon optimization was integrated into predictive control, which allowed the predicted sliding mode state to follow the expected trajectory of a predefined continuous convergence law. This scheme enabled the system to obtain higher output error accuracy and explicitly handle input constraints. Moreover, to enhance robustness, a parameter update law and disturbance delay estimation algorithm were introduced to calculate the control gain and total uncertainty, respectively. Finally, a comparative test of the proposed control scheme was conducted using a CRH380A HST simulation experimental platform in a laboratory setting. Simulation results demonstrate that the velocity error range of each power unit of the HST under the proposed control scheme is within [−0.176 km/h, 0.152 km/h], while the control force and acceleration are within [−55.7 kN, 44.8 kN] and [−0.564 m/s2, 0.496 m/s2], respectively, with stable variation, and other performance indicators are also better than other comparison methods. These results satisfy the safety, stability, and punctuality requirements of the train.