Police did not identify those arrested, but a person who had been briefed on the details said Brooks and her husband, a prominent horse breeder and a friend of Prime Minister David Cameron, were arrested at their house.
The six people were arrested on suspicion of conspiracy to pervert the course of justice, police said in a statement. The charge is an indication that investigators may be focusing on a possible cover-up of the scope of phone hacking.
The investigation stems from widespread wrongdoing at Rupert Murdoch's now-closed News of the World tabloid. The victims have ranged from celebrities and major politicians to the families of crime victims.
The Metropolitan Police said five men and a woman were arrested in various locations in and around London in a series of raids conducted between 5 am and 7 am on Tuesday.
Police said a 43-year-old woman was arrested at her home in Oxfordshire and is being questioned there.
Also arrested were a 49-year-old man in Oxfordshire, a 39-year-old man in Hampshire, a 46-year-old man in West London, a 38-year-old man in Hertforshire and a 48-year-old man in East London.
A judge-led inquiry into media ethics has heard extensive testimony about wrongdoing by tabloid journalists, and Murdoch's company has reached cash settlements with a number of victims.
There is also a simultaneous investigation into corrupt relations between the police and the press which has yielded a number of arrests in recent weeks.
An inquiry panel appointed by Prime Minister David Cameron is trying to determine why an initial police investigation into phone hacking in 2006 failed to reveal the scope of the problem.
At the time, Murdoch's executives claimed the wrongdoing was limited to one scurrilous reporter and an unprincipled private detective, both of whom were jailed.
The dormant police investigation was reopened last year after reporters were found to have hacked into the voicemail of a missing schoolgirl who was later found to have been murdered.
That investigation led to the resignation of Cameron's top media adviser, Andy Coulson, who had been the editor of the News of the World.
It also led to the arrest of senior Murdoch executive, the 43-year-old Brooks, who was later released on bail. Both have denied wrongdoing.
Murdoch's company has reached cash settlements with various hacking victims, including actress Sienna Miller and singer Charlotte Church, but many new cases are being brought against News International, the UK newspaper branch of Murdoch's global media empire.
The scandal also scuttled Murdoch's plans to purchase full control of the British broadcaster BSkyB.
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