This book provides a comprehensive exploration of AI-driven approaches to strengthening CPS security. Cyber-physical systems (CPSs) form the foundation of modern infrastructure, connecting physical processes with digital intelligence across domains such as health care, manufacturing, energy, and transportation. While CPS enables efficiency and innovation, their growing complexity also exposes them to significant cybersecurity risks. Artificial intelligence offers powerful solutions to these challenges, enabling intelligent monitoring, anomaly detection, intrusion prevention, and secure communication. Covering fundamentals, recent advances, and real-world applications, the chapters discuss threats, AI-enabled threat detection, anomaly detection in flexible manufacturing, machine learning for CPS resilience, and secure communication frameworks. Practical case studies further demonstrate the integration of AI in securing critical systems. With its interdisciplinary perspective, the book will benefit researchers, practitioners, and policymakers, offering insights into AI-based methods and future directions for creating intelligent, secure, and resilient CPS.