Rebekah Brooks and her husband are among six people who have been arrested by police investigating phone hacking.
The former News International chief executive has already been arrested under Operation Weeting, the Metropolitan Police's investigation into phone hacking at the company.
Five men and one woman were arrested at addresses in London, Oxfordshire, Hampshire and Hertfordshire between 5am and 7am on Tuesday morning on suspicion of conspiracy to pervert the course of justice.
Brooks and her husband are being interviewed separately at police stations in Oxfordshire and Buckinghamshire.
Director of group security at News International Mark Hanna, is also among the six suspects, according to the company.
A police spokesperson said: "All six - five men and one woman - were arrested on suspicion of conspiracy to pervert the course of justice, contrary to the Criminal Law Act 1977. A number of addresses connected to the arrests are being searched.
"Today's operation follows consultation with the Crown Prosecution Service."
Operation Weeting is running alongside Operation Elveden, which is looking into inappropriate payments to those in public life and Operation Tuleta, which is looking into computer hacking. The probe was set up in January 2011, the second police investigation into allegations of phone hacking at the News of the World.
So far there have been 22 arrests under Weeting.
The arrest of Charlie and Rebekah Brooks could potentially embarrass prime minister David Cameron, who has described Charlie as a "good friend." Cameron was recently forced to admit he had ridden a police horse loaned to Rebekah earlier this month, saying: "I've known Charlie Brooks for over 30 years and he’s a good friend, he’s a neighbour... I haven't been riding with him since the election.
“I have not been riding with him since the election. Before the election, yes, I did go riding with him."
"He has a number of horses and, yes, one of them was this former police horse Raisa, which I did ride.
Asked about the arrests on Tuesday a Downing Street spokesperson said: "The Prime Minister is travelling to Washington. It is an operational matter for the police. You wouldn't expect him to comment on it."
Rebekah Brooks' lawyer said last week that evidence given by Sue Akers to Leveson, the senior policewoman in charge of investigations into phone hacking, which claimed there was a "culture" of illegal payments at The Sun could prejudice any future trials.
Writing in the Daily Telegraph, Stephen Parkinson said: "There is no excuse for the spectacular failure that occurred.. "Witnesses have been summoned before both parliamentary committees and the Leveson Inquiry. As a result, much prejudicial material has come into the public domain."
Responding to the arrests shadow culture secretary Harriet Harman MP said the Leveson inquiry should look at "the full extent" of relationships between David Cameron and News International executives.
“Rebekah and Charlie Brooks are, on the prime minister’s own account, close friends of his.
“The Leveson Inquiry – when looking into the relations between the press and politicians – will need to investigate the full extent of the relations between the prime minister and senior News International executives at the time when hacking was rife and at the time his government was considering News Corp’s bid for BSkyB.”Suggest a correction