The couple welcomed son Knox Leon and daughter Vivienne Marcheline in France last month and subsequently sold the rights to the first pictures to America's People magazine for an estimated $11 million (GBP5.5 million).
In the new photo spread Pitt and Jolie are seen embracing the new additions to their family, while their two-year-old biological daughter Shiloh is pictured holding her baby sister.
The pair already has three adopted children Maddox, six, Pax, four, Zahara, three, and biological child Shiloh - and the twins extend their brood to six.
And Jolie insists that having such a large family is proving to be quite a struggle.
She says, "It is chaos, but we are managing it and having a wonderful time."
However, Jolie admits that she is getting some help with the babies - from her two elder daughters.
She adds,"(Shiloh) and Z (Zahara) pick out (the twins') clothes and help change and hold them. It's sweet - they are little mommies."
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