Media baron Rupert Murdoch's aide and the former editor of the News of the World, Rebekah Brooks, and her husband Charlie were arrested on Tuesday along with four others in connection with the phone hacking scandal.
Brooks, 43, a former editor of The Sun, had been on bail after being questioned by detectives last summer on suspicion of phone hacking and corruption, The Telegraph reported.
Police arrested six people at addresses in London, Oxfordshire, Hampshire and Hertfordshire.
The five men, aged between 38 and 49, and Brooks were arrested on suspicion of conspiracy to pervert the course of justice.
The coordinated arrests were made between 5 am and 7 am by officers from Operation Weeting, the Metropolitan Police's investigation into the illegal
This takes the total number of arrests under Operation Weeting to 23.
The probe was launched in last January after the police received new information from News International, the publishers of the News of the World, the Sun, the Times and the Sunday Times.
Previous arrests under Operation Weeting include Ian Edmondson, the former News of the World assistant editor; Neville Thurlbeck, the former chief reporter; Neil Wallis, the former executive editor; Rebekah Brooks, the former News International chief executive; and Stuart Kuttner, the former managing editor.
Previous Operation Weeting arrests for conspiracy to pervert the course of justice include Cheryl Carter, the long-standing assistant to Rebekah Brooks; Glenn Mulcaire, the private investigator; and Ross Hall, the former NOTW reporter.
