Barrymore and Kopelman, 39, began dating in February 2011 after being friends for a number of years and tied the knot in 2012.
In April they announced their split and offered an exclusive joint statement to WHO, and explained their daughters would always remain their first priority.
“Sadly our family is separating legally, although we do not feel this takes away from us being a family," they said. "Divorce might make one feel like a failure, but eventually you start to find grace in the idea that life goes on."