"After seven years, the opportunity from ITV felt like the right one to take," McCall said in a company statement of her switch to the British independent channel.
"It is a fantastic company in a dynamic and stimulating sector," she added.
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EasyJet said a search for McCall's successor had begun.
"Carolyn built and led the management team that has transformed EasyJet's performance in every respect since 2010," company chairman John Barton said in the statement.
"Having first built a solid operational performance, she redefined the customer experience not just at EasyJet but across short-haul Europe and has seen both the number and loyalty of EasyJet's passengers grow as a result," he added.
On her appointment at ITV, the group's chairman Peter Bazalgette said in a statement: "In a very impressive field of high calibre candidates, Carolyn stood out for her track record in media, experience of an international operation, clear strategic acumen and strong record of delivering value to shareholders."
Prior to become CEO of EasyJet, McCall had been chief executive of Guardian Media Group.
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