Jolie, 36, arrived at the Halo Trust centre in Thornhill on Saturday morning with four of her six children in tow, and remained there until 6pm for a private briefing by senior staff.
She is a long-standing supporter of the charity and has most recently travelled to Cambodia and Sri Lanka to raise awareness of its work in mine-clearance, but this was her first time at its Scottish headquarters.
Guy Willoughby, co-founder and director of the trust, said: “We keep in close touch anyway as she is one of our main private donors. She came with four of her kids and they had a look at what landmines are and then headed off to play with my children for the rest of the day.”
Mr Willoughby added that Jolie spoke warmly of her time in Scotland and her desire to return.
He said: “She said she just loved it up here. I see they’ve put their house in Malibu up for sale, so perhaps they’ll be swapping Malibu for Milngavie. You never know.”