Moazzam Begg was among four people arrested under suspicion of Syria-related "terrorism" offences, West Midlands police said on Tuesday.
Begg was arrested at his home in Birmingham on suspicion of "attending a terrorist training camp" and "facilitating terrorism overseas".
The other three, a 36-year-old man from Shirley and a 44-year-old woman and her 20-year old son from the Sparkhill area of Birmingham, were arrested on suspicion of facilitating attacks overseas.
The homes of Begg and the others being held were being searched by the police and vehicles and electronic equipment taken away for forensic analysis.
Begg, 45, was held by the US government at Bagram detention center in Afghanistan then Guantanamo Bay for three years before being released without charge in 2005.
He was arrested in Pakistan in February 2002 suspected of being a member of armed group al-Qaeda. Begg had travelled to Afghanistan with his family in 2001, but left after the US invasion.
After being freed from Guantanamo and returning to the UK, Begg frequently spoke out about human rights abuses at Guantanamo Bay and founded Cageprisoners, a human rights organization that lobbies on behalf of those held at the high-security prison located in Cuba.
Concern has been mounting in Britain over the number of nationals travelling to Syria to help terrorists. Police fear they may become radicalized or attend armed training camps before returning to the UK where they could pose a security risk.
NTJ/BA