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Cook, head of the $2.4 trillion company whose iPhone has revolutionised personal communication, was on the pope's daily audience list. As is customary, the Vatican did not disclose what was discussed during the private conversation.
The 85-year-old pope has a mixed relationship with cellphones. Last year, he interrupted his general audience when an aide passed him a cellphone and took an urgent call from a senior Vatican official.
He often patiently allows people to take selfies with him.
But he has also regularly warned people against becoming slaves to cellphones and other forms of technology.
"Free yourself from the addiction to mobile phones," he told young people in 2019. "When you become a slave to your mobile phone, you lose your freedom."
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On other occasions, he has said it was sad that people use their cellphone at the dinner table or while attending Mass.