Brad and Angelina showed the world that they are still crazy about each other as they embraced and gazed at each other lovingly while two of their six children looked on.
The loved-up pair were all smiles as they played with their oldest children Maddox, 7, and Pax Thien, 4, in a playground outside the centre.
Loved-up: Angelina Jolie and Brad Pitt look happier than ever as they take their boys Pax and Maddox to visit a housing project in New Orleans
Pitt is part of a commitment to build 150 new homes in the city's Lower Ninth Ward.
The actor's Make It Right project aims to re-build the New Orleans community that was hardest hit by Hurricane Katrina.
Meanwhile Angelina recently admitted that she turned to her late mother Marcheline Bertrand for inspiration in her new movie.
The 33-year-old is tipped for an Oscar for her role as a mother desperately seeking her kidnapped son in Clint Eastwood's The Changeling.
Domestic bliss: The pair embraced while their two oldest children looked on
'My mother would fight that hard for her children,' said the star.
She says the role made her think about her own children, with her baby twins taking the number to six.
She said the movie made her 'confront my worst fear. It made me feel closer to my kids and grateful every night just to know where they are and that they're healthy'.
Happy families: The couple with four-year-old Pax
The couple's oldest son Maddox struggles with an umbrella as they tour the project
She added: 'Making the phone call [in the film], saying that my kid was kidnapped, was difficult. I don't even like saying it right now.'
Angelina also revealed that her children produce 'the greatest chaos'.
'They're constantly loud, constantly messy,' she said.
But she admits that she and Brad are eager to add to their family 'one way or another', referring to how they have three children from adoption as well as three from Angie's own childbirth.
Angelina took half of her extensive brood out for an afternoon stroll to the shops in New Orleans last week.
Holding on: Angelina, pictured with Maddox, says that her role as a mother whose son is kidnapped in The Changeling made her 'confront her worst fear'
Boys just wanna have fun: Maddox and Pax Thien play together
Walk about: Angelina Jolie takes three of her six children Shiloh, Pax and Zahara for a walk to a nearby store in New Orleans yesterday
Leaving three-month-old twins Vivienne and Knox at home with their seven-year-old brother Maddox, Angelina brought Pax Thien, four; Zahara Marley, three; and Shiloh Nouvel, two; to the local Verdi Mart.
Dressed in a floor-length black dress, Angelina was careful not to trip as she carried blonde-haired Shiloh, who was clutching her beloved pink blankie and wearing neon green Crocs.
With Angelina going for the feminine look in her gown, tomboys Shiloh and Zahara were dressed in coloured jeans, while big brother Pax went for the workmen-style in dungarees.
The cute quartet, closely followed by two security guards, stopped at the store to buy packets of Cheetos (a cheese-flavoured cornmeal snack) for the kids and some bottled water.
Snack time: The kids clutch their bags of Cheetos after mum Angelina brought them to a local store
Earlier that day, proud father Brad was spotted cycling around the city on his way to a business lunch at Creole restaurant Antoine's.
Wearing a fedora hat instead of a cycling helmet, the handsome star was clutching a notebook with a picture of U.S. Presidential candidate Barack Obama on it.
The superstar couple bought a £1.75million, six-bedroom 1830s house in New Orleans' historic French Quarter in early 2007 in a bid to help regenerate the area.
Apple of my eye: Angelina keeps an eye on two-year-old Shiloh as she carries her pink blankie
They returned to New Orleans on Monday for the first time since the spring after spending the weekend in New York.
The couple spent most of the year in Europe - renting the £35million Miraval Estate villa in the French hamlet of Correns, in the Provence region - before moving to Germany last month, where Brad is expected to remain for most of the year making his latest film.
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