The Hollywood heartthrobs will be here for a month from mid-October to shoot a movie based on American journalist Daniel Pearl, who was beheaded in Pakistan four years ago.
Jolie plays Mariane Pearl, wife of the American journalist, who wrote the book "A Mighty Heart", on which the film is based. The star couple will be accompanied by their three kids - Maddox, Zahara and Shiloh-Nouvel.
Pune scored over other locations for the shooting as the city's landscape and ambience resembled Karachi and Islamabad in Pakistan. Pune is the cultural capital of Maharashtra, a state known more for the city of Mumbai - the country's financial and entertainment capital and home to Bollywood.
The Film and Television Institute of India is also based in Pune.
According to well-informed sources, a team from Britain and Mumbai-based producer Kailashnath Surendranath and his wife Arti did bookings in a few hotels and service apartments in the city a month ago.
Amit Bhosale, director of Bhosale Constructions, a biggie in real estate, is looking forward to the stars' visit, as his bungalow could be one of the places the couple might shoot in.
"I am looking forward to the Hollywood stars' visit. I don't know where the couple will stay although a team came and saw our 30,000-sq-ft-bungalow," Bhosale told.
He did not rule out the possibility of the crew using the Abby's Palace, his father Avinash Bhosale's house, in Baner, an upmarket locality in the western part of the city for the film shoot. The lush green, picturesque land has a clubhouse, helipad and a hangar.
Bhosale said the team also visited another of his sprawling bungalow called Jijai, named after the mother of Maratha King Shivaji at Bhosale Nagar area. "I really cannot wait to meet the duo," he said, unable to control his excitement.
"I do not want to say anything at this moment please," is all that Gauri Naiknavare, director of Naiknavare Builders, who own huge service apartments called Seasons in downtown Aundh area, said.
However, sources confirmed that two floors with 18 spacious rooms have been booked for the technical crew of the film from Oct 6 for six weeks.
Although all of them are double rooms, the foreign crew will occupy one each only, the sources said, adding a large crew from Bollywood, who will also stay in the city, will assist in the shooting.
Gopan Krishnan, director (sales and marketing) of Hotel Le Meridien, a five-star hotel, said that over 100 rooms have been booked in all the big hotels in the city.
"We have booked five best suites for the film unit and three other rooms. They will be our very special guests. But we have no details who will be staying with us," Krishnan told, adding that an array of Hollywood stars have enjoyed their hospitality in the past.
The Taj Blue Diamond hotel has also booked about 40 rooms for the film crew. Sources confirmed that Jolie and Pitt's security manager had surveyed the hotel and then confirmed the bookings.
"It is great for the city and the youngsters will have a ball," said Tripurari Sharan, director of the Film and Television Institute of India. He added that many Hollywood stars have visited the sprawling lush green campus of the institute.
The impending visit has added more hype as the Jolie-Pitt starrer "Mr and Mrs Smith" was a box office hit across India a year ago.
Model Vahbiz Dorabjee said she and her friends were excited about the stars touching down. "We are using all our contacts to get close to them. The city is really happening and I hope I get to shake hands with the cute Brad," she added, giggling.
"All the guys and girls are going gaga. Everywhere the talk is about the Jolie-Pitt duo and the film. There is a kind of frenzy in the air and the excitement is palpable," said city-based fashion choreographer Shekhar Sable.
Said Sonali Thatte, a senior manager with Vascon Engineers Pvt Ltd, a 20-year-old construction company: "I am excited about their stay in the city. The event will add more value to the city. Indeed, the city has really become a hot destination for the film industry too. I hope I will get to see the duo at close range if not shake my hands with them as I am sure there will be some parties thrown for them in the city."