With their budget of around £25m and a wish list that includes a prime central London location (a savvy investment and handy meeting point when work sees both of you continually circumnavigating the globe), sufficient space for six kids and, for the vineyard-owning parents, a private wine cellar, Brad Pitt and Angelina Jolie have set their sights on a penthouse in Marylebone.

Ten years ago, that would have been an unlikely sentence. Marylebone was one of those cut-through areas of the West End whose most exciting draws were the Waitrose and Daunt Books on the high street. But things have gone mad in the past year or two, helped massively by what Galliard Homes call “the Firehouse effect” – referring to Andre Balazs’ Chiltern Firehouse, the hotel/restaurant that sees celebrities falling over each other to be papped there.

Now that properties can achieve £3,500 per square foot in Marylebone, the area is starting to reach Belgravia and Knightsbridge levels. Rents have also risen by 10 per cent since the Firehouse opened in February, according to Knight Frank, who say Marylebone is no longer simply prime but “super prime” due to the number of £10m-plus sales it has seen this year.

Another reason for the rich and famous flocking to the area is Galliard Homes’ The Chilterns, the first entirely new-build development in Marylebone in five years. There’s another £1 billion of residential development in the pipeline locally too, but it seems the Jolie-Pitts may not be looking further than The Chilterns’ £25m duplex penthouse, which comes with a designer £100,000 wine cellar and tasting room stocked with £100,000 worth of wine.

According to Galliard’s chairman Stephen Conway, the Hollywood power couple would also join “overseas royals, business tycoons and international artists” if they buy in The Chilterns. That’s some residents’ meeting. Throw in a few Russian oligarchs and, increasingly, Chinese, Indian and Arab multi-millionaires and it’s a profile that’s typical of who is spending £20m on a house in London these days.  

So with that £20m or so burning a hole in their pockets, where else could Brad and Angelina choose to buy?

1. They could follow the lead of friends George and Amal Clooney and bypass London altogether in favour of a quiet spot in the Shires – in the Clooneys’ case, it’s said, a listed £10m manor house in the Thames-side Berkshire village of Sonning. A similar sum – leaving them £10m for a London flat too – would buy them Bishopsheath, an stately new-build country house on the edge of Windsor Great Park and near Wentworth. There’s an indoor heated pool, a tennis court, four acres of gardens and a private airfield 20 minutes drive away. It’s on sale for £10.5m through Hanover Private Office.

2. But if Brad, who is something of a modern architecture aficionado, is set on being in the thick of London buzziness and has an investor’s eye for an up-and-coming area, he might like the £19.75m penthouse at Neo Bankside. Designed by architects Rogers Stirk Harbour + Partners and interior designers Studio Reed, this 7,080 sq ft duplex has 360 degree views that take in every London icon from its triple aspect double-height reception room, four bedrooms, two winter gardens and two private rooftop terraces. Residents can also make use of a 24 hour concierge service – useful when jetting home from a shoot the other side of the world – and a gym and wine cellar.

3. Sticking to the South Bank and another architectural one-off, there’s the Dara Huang duplex penthouse on the 39th and 40th floors of the South Bank Tower – the old Kings Reach Tower that has now been turned into a luxury development of 191 apartments. The newly-opened Mondrian London hotel next door could well have the Chiltern Firehouse effect locally. The penthouse’s interiors comes fully furnished with bespoke interiors, inspired by contemporary art, and there are incredible Thames views. £20m, Savills, southbanktower.co.uk.

4. For classic Grade II-listed white stucco elegance and a prime establishment address, there’s 74 Chester Square, on sale for £23.995m (knightfrank.co.uk). The six bedroom, 6,291 sq ft house in a renowned Belgravia square has been newly refurbished and overlooks the residents’ private gardens. At the end of the street is village-like Elizabeth Street’s high-end boutiques and restaurants.

5. 43 Reeves Mews, two Edwardian mews houses knocked into one is now “Mayfair’s most outstanding ultra-prime residence”, says Peter Wetherell of Wetherell estate agency, who is marketing the house for £24m. The houses once belonged to the Le Mans “Bentley Boys” of the 1920s and converted by developer Fenton Whelan into a seven-bedroom house that includes huge entertaining rooms, cinema, gym and staff quarters. The architectural centrepiece is a spiral staircase that weaves its way from lower ground to the top floor. Above is a glass cupola from which hangs a bespoke three-storey drop, 350kg Bohemian crystal chandelier.

6. Treetops on Compton Avenue, N6, is a newly-built 10-bedroom house spanning over 16,000 sq ft next to Highgate Golf Course and set opposite Hampstead Heath. Features include indoor and outdoor swimming pools, cinema, car lift and two-bed staff apartment. On sale for £24m through Glentree Estates.

7. The quirkiness of The Red Brick House in Little Venice, W9, might appeal to Brangelina. So too will the fact that the house was built in 1929 by Scottish architect Charles Stanley Peach, a follower of Rennie Mackintosh (Pitt is a patron of the charity to raise funds for the Mackintosh library rebuild in Glasgow). This intricately adorned five-bed house has all the five-star amenities a Hollywood family could ask for, including pool, bar and cinema, and it comes with a separate three-bed mews house for the kids. It’s on sale for £17.95m through Aston Chase.