This two-volume set LNICST 396 and 397 constitutes the post-conference proceedings of the Third EAI International Conference on Artificial Intelligence for Communications and Networks, AICON 2021, held in September 2021. Due to COVID-19 pandemic the conference was held virtually. The 79 full papers were carefully reviewed and selected from 159 submissions. The papers are organized in topical sections on Artificial Intelligence in Wireless Communications and Satellite Communications; Artificial Intelligence in Electromagnetic Signal Processing; Artificial Intelligence Application in Wireless Caching and Computing; Artificial Intelligence Application in Computer Network.