The chef, who holds two Michelin stars at Notting Hill's Core by Clare Smyth, will launch a project at the high-rise property in February 2021.
While the restaurant will draw inspiration from Core, Smyth plans to create a unique experience reflecting local produce.
Smyth's restaurant will be one of 14 food and beverage outlets set to open at the Barangaroo development, which includes a 349-room hotel.
Several international chefs are due to collaborate on projects at the site, though Smyth is the first to be announced.
“Crown Sydney is creating a world-class dining destination for the city, and I am thrilled to have my first Australian restaurant in this amazing location overlooking one of the most beautiful sites in the world,” says Smyth.
“With this new restaurant I wish to build upon the success of Core. Having lived and travelled in Australia early on in my career, it feels like a home away from home and the perfect location for the restaurant.”
Smyth trained in restaurants including Alain Ducasse’s Le Louis XV in Monaco and spent 13 years at Restaurant Gordon Ramsay, where she became the first British woman to oversee a restaurant holding three Michelin stars.
Core opened in 2017 and has won plaudits for its elegant dishes celebrating British produce. In 2019 it was ranked fourth in Restaurant magazine's list of the top 100 restaurants in the UK, and 66th in the World's 50 Best Restaurants longlist.
Smyth has appeared on Network Ten’s Masterchef Australia, as well as Netflix’s Final Table.