A senior security man at News International was understood to be among those held yesterday, after victims of phone hacking obtained evidence of the systematic deletion of compromising emails and the destruction of computers used by News of the World staff.
Mr and Mrs Brooks were at their home in the Cotswolds, expecting to head off to Cheltenham when they were arrested between 5am and 7am.
In January the couple became parents of a surrogate daughter, Scarlett Anne Mary Brooks, who was born at the Portland private hospital in central London.
They could have been forgiven for thinking they would be spending a few days relaxing, especially after the recent “horsegate” disclosure that Scotland Yard lent a retired police horse to Mrs Brooks, which David Cameron had ridden.
Instead, they both found themselves under arrest for an offence that could potentially have far worse implications than the phone hacking which allegedly took place on Mrs Brooks’s watch.
Mr Brooks, 49, was not even married to the former News of the World editor at the time the hacking was allegedly going on, but he came to the attention of police when his laptop was handed in to police the day after his wife’s arrest last July.
Officers from Operation Weeting, the investigation into phone-hacking, and Operation Elveden, the investigation into illicit payments to public officials, had spent nine hours questioning Mrs Brooks on July 17, two days after she resigned as chief executive of News International. She has been on bail since.
The following day a laptop computer and an iPad belonging to Mr Brooks were handed in to police by a security guard at the Design Centre apartment complex in Chelsea Harbour, west London, where Mr and Mrs Brooks have a £1.5 million flat.
A bag containing the computers, a phone and some paperwork had been found in an underground car park by a cleaner and dumped in a bin, where it was found by the security guard.
Mr Brooks said at the time that his briefcase had been dropped off and “there was a misunderstanding about collecting them by a mate”.
He told The Daily Telegraph he was “glued to Sky News” at the time, and that the briefcase “ended up with the trash”.
He added in an email that it was “all my personal info, nothing to do with my wife or search warrant”.
He said he had contacted the police when he realised the bag was missing, and that they confirmed the items had been handed in.
Mr Brooks was taken to a police station in Buckinghamshire yesterday while his 43-year-old wife was taken to a police station in Oxfordshire.
She is likely to have been questioned over disclosures in recent weeks about the deletion of emails and the destruction of computers used by News of the World reporters, which emerged during High Court hearings at which dozens of hacking victims accepted damages from the publisher of the defunct newspaper.
Mrs Brooks was editor of the tabloid from 2000-2003, then served as editor of The Sun until Sep 2009, when she became chief executive of News International.
Last month The Daily Telegraph disclosed that executives at News Group Newspapers had formulated an “email deletion policy” in November 2009 to “eliminate in a consistent manner” emails that could cause trouble.
Staff were told to destroy emails that “could be unhelpful in the context of future litigation in which a News International company is a defendant”.
Papers released by a High Court judge showed that hundreds of thousands of emails were deleted “on nine separate occasions”. One senior executive told a member of staff to remove seven boxes of paper records from the company’s storage facility, it emerged.
Lawyers for some of the hacking victims told the High Court at a separate hearing that computers used by News of the World journalists implicated in the hacking scandal were destroyed in 2010 as part of a “conspiracy” to cover up the extent of phone hacking and the identities of those who knew about it.
Mr Justice Vos, who is presiding over the hacking cases, said he had seen evidence that raised compelling questions about whether News Group “concealed, told lies, actively tried to get off scot free”.
Four men, aged 39, 46, 38 and 48 were arrested in co-ordinated raids in Hampshire, Hertfordshire and London, taking the total number of arrests under Operation Weeting to 29.
A spokesman for Mrs Brooks declined to comment.