"We are confirming that the individual who was asked to leave the country last week is no longer in Germany," a US embassy spokesman said.
A German foreign ministry spokesman also confirmed the news that the US spy chief had left.
The daily Sueddeutsche Zeitung cited German and US government sources as saying that the man took a commercial flight from the western city of Frankfurt bound for the United States.
Germany last week ordered the CIA station chief out of the country amid the worst diplomatic row between the close NATO allies since the US-led invasion of Iraq in 2003, which Berlin vocally opposed.
More From This Section
Federal prosecutors are investigating a defence ministry employee and an agent for the BND foreign intelligence agency on suspicion of supplying secrets to Washington.
The cases stoked still seething anger in Berlin about revelations that the US National Security Agency conducted mass spying operations against targets including Merkel's mobile phone.
Merkel and US President Barack Obama spoke by telephone Tuesday for the first time since the expulsion order against the CIA chief.
A White House statement said little about the conversation, only that Obama and Merkel "exchanged views on US-German intelligence cooperation, and the President said he'd remain in close communication on ways to improve cooperation going forward."
In a interview with public television last Saturday, Merkel lamented the breakdown of trust between Germany and the United States and a return to the thinking of the "Cold War era where everyone is suspicious of everyone".
US Secretary of State John Kerry attempted to mend fences Sunday at talks with his German counterpart Frank-Walter Steinmeier in Vienna, insisting that the transatlantic allies remain "great friends".