"We must... Continue to confront state actors whose influence fuels instability in the region," May told Gulf leaders at the summit.
"So I want to assure you that I am clear-eyed about the threat that Iran poses to the Gulf and to the wider Middle East."
She added: "We must... Work together to push back against Iran's aggressive regional actions."
May said she wanted a "strategic partnership" to help boost security in Gulf countries, including defence investment and military training in Bahrain and Jordan.
"I want these talks to pave the way for an ambitious trade arrangement" after Brexit, she said.
King Salman of Gulf heavyweight Saudi Arabia opened the summit on Tuesday with a call for a "doubling of efforts" to face regional challenges.
In October last year, Britain began building a naval base at Mina Salman, outside Manama, its first new permanent base in the Middle East in four decades.
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