Germany's BND intelligence service eavesdropped on high-placed French civil servants at the Elysée presidential palace, the French Foreign Ministry and the European Comission, according to the Sueddeutscher Zeitung.
Earlier this week it was revealed that the BND had tapped phones and emails of French-based companies at the request of the NSA, which in turn had spied on German leaders, including Chancellor Angela Merkel, according to documents leaked by whistleblower Edward Snowden.
The Sueddeutscher Zeitung says that was limited because the Americans wanted information on illegal exports.
"The heart [of the problem] is political espionage of European neighbours and institutions of the European Union," the paper claims, citing a source with knowledge of BND's procedures.
European Commission head Jean-Claude Juncker said he expected Germany to establish the truth.
"I know from personal experience that [the secret services] are very difficult to be kept under control," the former Luxembourg prime minister said. "The German authorities will have to deal with that and I expect they will."
Germany's current Interior Minister Thomas de Maiziere, who was chief of staff at the Chancellor's Office from 2005-2009, has promised to provide an explanation to a parliamentary commission looking into the revelations.
But the opposition has accused the government of lying when it denied any knowledge of the economic espionage.