Understanding the dynamic behavior of tires and their interactions with roads plays an important role in designing integrated vehicle control strategies. Accordingly, having access to reliable information about tire–road interactions through tire-embedded sensors is desirable for developing enhanced vehicle control systems. Thus, the main objectives of this research are: 1) to analyze data from an experimental accelerometer-based intelligent tire acquired over a wide range of maneuvers, with different vertical loads, velocities, and high slip angles and 2) to develop a lateral force predictor based on a machine learning tool, more specifically, the Gaussian process regression (GPR) technique. It is determined that the proposed intelligent tire system can provide reliable information about the tire–road interactions even in the case of high slip angles. In addition, lateral force models based on GPR can predict forces very well, outperforming other machine learning models and providing levels of uncertainty that can be useful for designing vehicle control strategies.