"Twenty fire engines and around 125 firefighters are now responding to the fire at Somerset House. Crews are continuing to work at bringing the fire in the building's roof under control," the London Fire Brigade posted on X, formerly Twitter.
The official X account of the Renaissance building, which opened in 1796, said that "owing to a fire in one small part of Somerset House, the site is currently closed."
It added that "all staff and public are safe."
The complex is home to the Courtauld Gallery, which houses priceless paintings, including Vincent van Gogh's "Self-Portrait with Bandaged Ear."
Other footage taken from central London showed thick plumes of smoke rising above the building, which stretches for around 180 metres along the banks of the River Thames.
The courtyard of the grand building hosts music gigs in the summer and a popular ice rink in the winter, appearing in the 2003 film "Love Actually".
It has also appeared in two James Bond films, the 2008 movie "The Duchess", starring Keira Knightley and Ralph Fiennes, and Tim Burton's 1999 horror movie "Sleepy Hollow".
The fire service said two 32-metre ladders had been sent to the scene to support firefighting operations.
"The entire site at Somerset House is now closed to the public whilst we tackle the fire. Traffic in the surrounding area will be impacted as crews respond," it added.
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