The 53-year-old actor - who split with Angelina in 2003 after three years of marriage – says he only remembers the positive aspects of their relationship and has the ‘utmost respect’ for the 33-year-old.
‘I've never said anything but good things about any relationship I've had and, frankly, that's all I remember about them.
Still in touch: Billy Bob Thornton's disclosure that he and Angelina are still close is bound to trigger fresh tension in Pitt and Jolie's reportedly strained relationship
‘I have the utmost respect for Angelina. She's a very sweet person, very talented and one of my best friends in the world,’ he told Parade.com
The star’s comments look set to cause further tension between Jolie and her partner Brad Pitt, who have been plagued by split rumours in recent weeks.
Jolie’s friendship with Thornton has long been the cause of friction between the pair, according to US reports, with Pitt said to disapprove of the pair's on-going relationship.
Stiill close: Angelina with former husband Billy Bob Thornton in 2001
Meanwhile a miserable Pitt visited the doctor in Germany alone today for an undisclosed medical condition.
There has been no sign of Jolie and their six children since the actor arrived in Berlin.
The Jolie-Pitt clan are moving to the city after six months in France, where Jolie gave birth to the couple's twins in July.
Where's Angie? A sombre Brad Pitt ventures out alone in Berlin last night, amid rumours his relationship with Jolie is in crisis
As they prepare to live in Berlin for the remainder of the year while Pitt films his latest movie Inglorious Bastards, sources say the relationship between the couple is at breaking point.
Despite the couple issuing a denial they were splitting last week, friends of the pair say there has been a build up of tension between them over the past few weeks.
Tension: Angelina Jolie is said to be upset with the amount of time Brad Pitt has spent away from the family in recent weeks
Pitt, 44, has spent a lot of the past month abroad promoting his new film Burn After Reading at the Venice and Toronto Film Festivals, while Jolie has been at the couple's new home in France with their six children, including their two-month-old twins.
At the Toronto Film Festival two weeks ago, Pitt was rumoured to have met his ex-wife Jennifer Aniston for a lunch date as they were both in the Canadian city promoting their new movies at the same time.
After returning to France, Pitt then flew 600 miles away from their home on the Riviera to Normandy to film a Japanese cellphone commercial, reportedly leaving Jolie fuming.
Family man: Pitt with his two oldest sons Maddox and Pax in Venice last month
A source tells America's Star magazine: 'Things have gotten heated between Angie and Brad. Angie is volatile right now. She misses her mother (who died last year) more than ever, she's barely eating and she feels stuck at home amid total chaos with six kids.
'And to make matter worse, she's nagging Brad to the point that he uses any excuse to take off.'
American magazine In Touch Weekly reported Jolie grew so angry with Pitt, she threatened to end their relationship, which prompted the split reports last week.
A source said: 'She told Brad they were over. She said she didn't want to be with him any more and she wanted to split.'
Last week, the magazine reported Jolie was suffering from post-natal depression following the birth of the twins and this had been causing a strain with Pitt.
An insider explained: 'He's grown used to her mood swings, so he just tries to stay cool.
'If she doesn't want to see him, he stays away, but it break his heart not being around the kids.'
Last year, Jolie, 33, complained the couple barely had any alone time because they were so busy with the children.
She told Marie Claire magazine: 'Mommy and Daddy need to try to figure out more time right now.
'We're working on it; we're working on it. Right now, we're not great about Mommy-and-Daddy time.'
When the couple first started dating in 2005, they had to balance getting to know each other with caring for Jolie's son Maddox - who Pitt later adopted - and welcoming newly adopted daughter Zahara into the family.
The couple now have three adopted children and three biological children in total - Cambodian Maddox, seven; Ethiopian Zahara, three; Vietnamese Pax Thien, four; Shiloh Nouvel, two; and twins Knox and Vivienne, 10 weeks.
The lakeside mansion: It is reported that Brad and Angelina are to move their family to the Palais Schlosspark in Berlin
The huge house stands on the shore of Lake Wannsee
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