The sultry ex-Supermodel — who has campaigned widely against AIDS — accused the Catholic Church of "damaging" Africa with its views on birth control.
Italian-born Carla is so furious she revealed she no longer practised the religion.
Her outburst, made at the Elysee presidential palace in Paris, has caused uproar among the country’s millions of Catholics.
Angry Carla said: "I was born Catholic, I was baptised, but in my life I feel profoundly secular.
"I find that the controversy coming from the Pope’s message is very damaging.
Astonishing
"In Africa it’s often Church people who look after sick people. It’s astonishing to see the difference between the theory and the reality.
"I think the Church should improve on this issue. It presents the condom as a contraceptive which, by the by, it forbids, although it is the only existing protection."
The attack, made to women’s magazine Femme Actuelle, is sure to upset Carla's husband, President Nicolas Sarkozy, who previously told the public he was of "Catholic culture, Catholic tradition, and Catholic faith".
Religious groups in Paris were quick to condemn Miss Bruni.
Notre Dame Cathedral parishioner Jean Martin blasted: "It is not the job of a First Lady, especially one who is a baptised Catholic, to attack the Pope. Such words bring shame on the presidential office."
Historian Jean-Luc Deloire said: "There is a long-standing tradition in France that the First Lady keeps her counsel. Attacking anybody, least of all the Pope, should not be on the agenda."
Carla is a highly controversial figure in France, as her ex-lovers include rock stars Mick Jagger and Eric Clapton and a number of other public figures.
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