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The actor was snapped sharing an ice cream cone with grandchildren Pax and Zahara as they walked in a London park.
Pitt and Jolie were reportedly not present for the outing because they are currently both working on upcoming films.
Jolie and Voight's relationship has been notoriously rocky, but the stars reconciled in 2009 after not speaking for nearly eight years.
In September 2010, Voight praised Jolie's children as "beautiful" and extremely smart.
Jolie revealed this week that she and Pitt are not organising a "secret wedding" and have no plans to adopt more children for the time being.
> Angelina Jolie, Brad Pitt household has "calmed down"
> Angelina Jolie visits anti-landmine charity in Scotland
Watch Angelina Jolie in the trailer for The Tourist below:
