The videos, released as part of a Freedom of Information Act, show members of a ring of Russian sleeper spies surreptitiously passing information and money.
The tapes include footage of former New York real estate agent Anna Chapman, whose role in the spy saga turned her into an international celebrity. She bought leggings and tried on hats, investigators said, and transmitted coded messages while sitting in a downtown coffee shop in New York City in January 2010.
Other footage shows some of the 10 other conspirators burying money in a patch of weeds, handing off documents in what looks like a subway tunnel, meeting during a stroll around Columbus Circle or just taking their kids for a walk.
The FBI also released more than 1,000 pages of highly redacted documents from the operation dubbed "Ghost Stories" because it was reminiscent of the Cold War's cloak-and-dagger spy games.
FBI agents and the Justice Department arrested the 10 spies on June 27, 2010. The spies were then swapped on July 9 for four Russians who were imprisoned for spying for the West.
Called illegals because they took civilian jobs instead of operating inside Russian embassies and military missions, the spies settled into quiet lives in middle-class neighborhoods.
Their long-range assignment from Moscow was to burrow deep into U.S. society and cultivate contacts with academics, entrepreneurs and government policymakers on subjects from defense to finance.
President Dmitry Medvedev awarded all 10 of the freed deep-cover operatives with Russia's highest honors at a Kremlin ceremony.
Chapman went on to become a lingerie model, corporate spokeswoman and television personality.
ABC News and the Associated Press contributed to this report.