St James's Court, which used to be a Crowne Plaza hotel, originally opened in 1902 and has regularly hosted royalty and Heads of State. It has four event spaces and 13 meeting rooms.
The Taj Group has also rebranded the Taj 51 Buckingham Gate, Suites and Residences, which will welcome a new lobby and reception lounge, a new restaurant, tea and library lounges and an exclusive private dining area in 2014.
Both hotels will provide complimentary wi-fi, a wellness centre and a host of on-site dining options, including Michelin-star Quilon.
Raymond Bickson, managing director and chief executive officer of the Taj Group, said: "This important re-branding comes at an exciting time for the increasing strategic links between India and UK. We are delighted to have the opportunity to restore these iconic hotels that have more than a century of heritage."
Deepa Harris, senior vice president of global sales and marketing of the Taj Group, added: "The success of our London hotels provided the impetus to consolidate our brand presence in the UK, being an important source market for Taj.
"St. James' Court, A Taj Hotel is positioned as an English classic, while Taj 51 Buckingham Gate Suites and Residences will offer authentic luxury experiences."