The 'Maleficent' actress - who married the 52-year-old actor in the South of France in 2014 after 12 years of dating - allegedly barely uttered a word to her spouse whilst they spent their honeymoon filming 'By The Sea'.
According to PEOPLE the couple - who have only been married two years and are in the middle of a divorce - showed visible signs of tensions when they shot scenes for the drama film in Malta.
A source said: "They hardly spoke when they were together.
"He would be very quiet and just keep to himself.
"It was not a honeymoon."
Although the 41-year-old directed and starred in the movie alongside her estranged husband, she reportedly "never" spent any time with him.
The source added: "Angelina was never with him."
However, the tension has continued as it has recently reported there is a lot of "bad blood" between the Hollywood couple, which has left Angelina "seething" at her partner.
Although Brad is "frustrated" with Angelina - who has recently been granted full custody of her children in a temporary custody deal with Brad, which will see her have full physical custody of her children for three weeks until October 20 when new recommendations can be settled - and reportedly has "so much stuff" on her that he could use against her, he won't bring any of it up in the court battle because he doesn't want to "play dirty".
Speaking previously, a source said: "There is so much stuff on Angelina but Brad just doesn't want to go there. He told his team he doesn't want to play dirty.
"Brad just wants to work through everything and get to a place where there can be some certainty about what's going on. The kids are the only thing he's hanging on to."