The agenda of Industry 4.0 highlights smart manufacturing by making machines smart enough to make data-driven decisions. Large-scale 3D printers, being one of the important pillars in Industry 4.0, are equipped with smart sensors to continuously monitor print processes and make automated decisions. One of the biggest challenges in decision autonomy is to consume data quickly along the process and extract knowledge from the printer, suitable for improving the printing process. This paper presents the innovative unsupervised learning approach, bootstrap–CURE, to decode the sensor patterns and operation modes of 3D printers by analyzing multivariate sensor data. An automatic technique to detect the suitable number of clusters using the dendrogram is developed. The proposed methodology is scalable and significantly reduces computational cost as compared to classical CURE. A distinct combination of the 3D printer’s sensors is found, and its impact on the printing process is also discussed. A real application is presented to illustrate the performance and usefulness of the proposal. In addition, a new state of the art for sensor data analysis is presented.