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Overton, 43, will handle a broad range of issues for Goldman, a spokesman for Goldman said.
Overton spent less than two years at Citigroup, and previously worked as counsel to Senator Tom Carper, a Democrat of Delaware, during negotiations for the Dodd-Frank Act.
"Amy's long experience with financial services issues will make her a great addition to our team," said Michael Paese, head the Washington government relations office for Goldman Sachs. Overton will report to Paese, and will have the title of vice president, the same title she had at Citigroup.
A Citigroup spokeswoman declined to comment.
Overton also worked at Fannie Mae FNMA.OB for seven years leading into the financial crisis, leaving as chief of staff for its government and industry relations department in 2008.
With Overton's joining, Goldman's D.C. office is now evenly split between Democrats and Republicans, with four of each.
Paese had been a top staffer for former Democratic congressman Barney Frank. Goldman's lobbying office has two other Democrats, said a person familiar with the matter who did not have authorization to speak publicly about the matter.
Todd Malin, a senior Republican lobbyist, recently left Goldman for Rio Tinto PLC (RIO.L). But the bank has other Republicans in its lobbying group, including global head of the office of government affairs, Faryar Shirzad, who splits his time among London, New York and Washington.
Reporting By Lauren Tara LaCapra; Editing by Leslie Adler