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He took advantage of the tumultuous reign of the pharaoh Akhenaton, and seized control of Egyptian territory in Syria, inciting many Egyptian vassals to revolt. His success encouraged the widow of the Egyptian king Nibhuruyiras (identified with either Akhenaton or Tutankhamun) to write to him, asking him to send one of his sons to be her husband, and rule Egypt. Suppliluliuma sent an ambassador to investigate, who reported that the situation was accurately described, and the king decided to take advantage of this windfall; unfortunately, prince Zananza died on the way, and the marriage alliance never was consummated.

Suppiluliuma also crushed the independent Mitanni kingdom ( Hanilgalbat), reducing it to a client state under his son-in-law Shattiwazza , and rebuilt the Hittite capital at Hattusas.

The Annals of Suppiluliuma, compiled after his death by his son Mursili, is an important primary source for the 14th century BC. One of Suppiluliumas' letters, addressed to king Huriya (most likely Smenkhkare, but also identified with Tutankhamun and Akenaton) was preserved in the Amarna letters (EA 41).