The iTrust datasets comprise cyber-physical security data from operational water infrastructure testbeds, primarily the Secure Water Treatment (SWaT) and Water Distribution (WaDi) systems, along with Critical Infrastructure Security Showdown (CISS) attack exercise data. They include time-stamped historian measurements from sensors and actuators, network traffic PCAP files, NetFlow logs, and labeled records of normal operations and cyber-physical attack scenarios. The data spans multiple collection periods, including long clean runs and attack campaigns involving process disruption, data exfiltration, and red-team attacks. These datasets support research and evaluation in industrial control system security, anomaly detection, attack detection, and machine-learning methods for protecting critical infrastructure.