Artificial intelligence (AI) can be a powerful tool in the management of critical systems that have traditionally been under human control. The EU-funded AI4REALNET project will develop methods to prioritise trustworthiness in AI-assisted human control, incorporating augmented cognition, hybrid human-AI co-learning, and autonomous AI, all while maintaining a focus on the resilience, safety, and security of critical infrastructures. The project will also expedite the development and validation of new AI algorithms by the consortium and the broader AI community. It will do this by leveraging open-source AI-friendly digital environments capable of simulating realistic scenarios involving the operation of physical systems and human decision-making. Finally, AI4REALNET will contribute to addressing the critical aspects of decarbonisation, digitalisation, and resilience.