The 42-year-old Oscar winner was seen leaving Heathrow with her daughter Shiloh (11) and son Knox (9).
Angelina's arrival has fueled speculation among the British public as to whether she'll attend the wedding of Prince Harry and Meghan Markle on Saturday.
Although Angelina has no known links with American actress Meghan Markle, she is said to be close to the royal family after being made an honorary dame by Britain's Queen Elizabeth last October.
The actress is said to be heading in and out of London to film the sequel to Disney's 2012 film Maleficent, according to The Daily Mail.
What celebrities are expected to attend the royal wedding?
As the week nears in to Harry and Meghan's big day, wedding fans have been dying to find out what celebrities will be in attendance on Saturday 19 May.
Hollywood royalty George and Amal Clooney are among the guests rumored to be attending Prince Harry's big day.
Amal's hairdresser Miguel Perez told Hola! Magazine that he would be in charge of doing Amal's hair for the wedding weekend.
Elton John, who was friends with Harry's mother Princess Diana, is said to be attending the wedding after cancelling two of his other concerts.
An official statement from the singer said the concerts on May 18 and May 19 were cancelled due to a 'scheduling error', but many fans believe he's preparing for the royal event instead.
Victoria Beckham recently confirmed her and husband David Beckham's attendance. The couple also attended the wedding of Prince William and Kate Middleton in 2011.
Victoria's former band mates in The Spice Girls are also rumored to have received an invite to the elite event, a source told US magazine.
Markle's co-stars in the hit TV show Suits have been spotted around the British capital. 46-year-old actor Gabriel Macht, who plays Harvey Spector, touched down in London last week.
Their co-star Sarah Rafferty, known as Donna Paulsen in the show, has posted pictures of herself on Instagram travelling around Europe in the lead up to the big day. The American actress was pictured arriving in London yesterday.