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Theodore Goddard is to become the third large firm to lose its private client practice in a month.
The department, comprising partners Joyce Smyth and Caroline Barkham and two assistants, will break away to set up on their own, Smyth Barkham, in Fleet Street on 1 May.
Smyth said the split was amicable and that they had jumped rather than being pushed. She said Theodore Goddard had not asked them to leave "but I felt they might have done in five years' time".
"We are just thinking ahead. I have been on TG's management board so I can see the way the big firms are going and we thought, it is time to do it."
Last month both Dibb Lupton Alsop and Eversheds lost private client departments, with Dibbs' London team going to Lawrence Graham while Eversheds' Birmingham team joined Martineau Johnson.
And in the past few years many of the larger City firms have either shed or down-sized their private client departments - the lawyers generally moving to smaller firms.
Freshfields cut back its private client work in 1990; McKenna & Co transferred its private client practice to Wilsons in 1991 and Richards Butler closed its department in the same year.
Withers & Co picked up Slaughter and May's private client lawyers in 1994 and Lovell White Durrant's private client department in 1995. In January this year Norton Rose offloaded its private client operation to Charles Russell.