Coulson, 44, is being held on suspicion of committing perjury at the trial of former MSP Tommy Sheridan in 2010.
Coulson was detained at his home in the Dulwich area of London at 06:30 by seven officers from Strathclyde Police.
However, Coulson has not been charges and is not under arrest.
Coulson is detained because in Scotland, a suspect is held on suspicion of an offence, unlike in England and Wales where a suspect is arrested.
In 2010 Coulson, former editor of the News of the World, provided evidence at the perjury trial of former Scottish Socialist MSP Tommy Sheridan.
Sheridan was awarded £200,000 in damages from the News of the World in 2006 after it printed allegations that he had committed adultery and visited a swingers’ club.
The former MSP and his wife Gail were charged with perjury.
She was acquitted during the subsequent trial but Sheridan was convicted in December 2010. After serving just over a year of a three-year sentence he has been freed.
Sheridan represented himself at the trial and questioned Coulson’s knowledge of any illegal activities, including phone hacking. Coulson denied all allegations.
During the trial he was employed as Prime Minister David Cameron’s director of communications.
However, in January 2011 Coulson resigned from that post, claiming the coverage of the News of the World phone hacking scandal was too distracting from his role.
Coulson was arrested in July 2011 by Metropolitan Police investigating the News of the World hacking scandal and later released on bail.
Sheridan’s solicitor, Gordon Dangerfield, will be lodging a full appeal in due course.
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