Following his turn on stage, the pair were spotted in the theatre’s coffee shop alongside Jolie’s 16-year-old daughter Shiloh.
The trio were seen sitting around a table chatting in a post that was shared on a fan Instagram page, @paulmescalpics.
Sharing the unexpected meeting on social media, the account wrote: “Angelina Jolie saw A Streetcar Named Desire yesterday and after they grabbed a coffee at the @almeida_theatre Cafe!
“Her daughter was there as well.”
It was also shared by other fan accounts.
In the photo, Mescal kept things casual wearing a red T-shirt while 47-year-old Jolie donned a black trench coat and Shiloh sported a cream beanie.
There has been speculation Mescal has split from musician Phoebe Bridgers.
Bridgers and the Irish actor sparked engagement rumours in April when it was reported by The Sun that the 28-year-old singer had referred to Mescal as her “fiancé” at Coachella.
However, the Kyoto hitmaker has set tongues wagging about a possible split after she and comedian Bo Burnham were spotted “canoodling and cuddling” at several locations in Los Angeles in recent weeks.
According to Deux U podcast, they were seen at local bar The Magic Castle and at a The 1975 concert, at which they posed for a photo that saw Bridgers playfully kissing the band’s frontman Matty Healy.
Bridgers and Burnham, who have been friends since 2021, furthered the dating speculation when they sat next to each other at Kate Berlant’s one-woman comedy show on Monday in New York.
Burnham, 32, is said to have given the singer his “undivided and doting attention” before the show, which he was directing, got cancelled due to technical difficulties.
“It felt flirtatious, like he was trying to impress her,” a reporter at Jezebel, who attended the gig, claimed. The Standard contacted reps for Mescal, Bridgers and Burnham at the time.