McCarry served in the United States Army, where he was a correspondent for Stars and Stripes, has been a small-town newspaperman, and was a speechwriter in the Eisenhower administration. From 1958 to 1967 he worked for the CIA, under deep cover in Europe, Asia, and Africa. However, his cover was not as a writer or journalist. He is married with four grown sons. His family is from The Berkshires area of western Massachusetts, where he currently lives.[

He is an admirer of the work of W. Somerset Maugham, especially the Ashenden stories. He was also an admirer of Richard Condon, author of The Manchurian Candidate, Prizzi's Honor and numerous other novels.

McCarry was editor-at-large for National Geographic and has contributed pieces to The New York Times, The Wall Street Journal, The Washington Post, and other national publications.

His novels are currently being reprinted by Overlook Press, starting with Tears of Autumn, republished in 2005. Charles N. Brown, the publisher of Locus, which primarily addresses the science-fiction publishing world, wrote in the July 2006 issue: "Two Charles McCarry hardcover reprints from Overlook... aren't really SF or fantasy, but they are two of the best spy thrillers ever written and form a secret or alternate history of the 20th century."

McCarry is best known for a series of books concerning the life of super spy Paul Christopher. Born in Germany before WWII of a German mother and an American father, Christopher joins the CIA after the war and becomes one of its most effective spies. After launching an unauthorized investigation of the Kennedy assassination, Christopher becomes a pariah to the agency and a hunted man. Eventually he spends ten years in a Chinese prison before being released and embarking on a solution to the mystery that has haunted him his entire life: the fate of his mother who disappeared at the beginning of WWII. The books are notable for their historical detail and depiction of spycraft, as well as their careful and extensive examination of Christopher's relationship with his family, friends, wives, and lovers.

Also notable are two books dealing with Paul Christopher's American cousins, Horace and Julian Hubbard: The Better Angels and Shelley's Heart. These novels tell the story of a U.S. President who approves the assassination of the leader of an oil-rich Arab nation who has acquired nuclear arms and intends to pass them onto a terrorist organization. When news of this threatens to ruin the President's chances for re-election, the Hubbards conspire to steal the election. In Shelley's Heart, the conspiracy is revealed and the newly re-elected President is impeached and placed on trial in the Senate. Both books indicate an extensive knowledge of Washington politics on the part of the author.

McCarry's most unusual book in the series, also concerning the Christopher family, is Bride of the Wilderness. Set in the 17th century, it's a historical romance concerning one of Paul Christopher's ancestors, the English-born Fanny Harding. After the death of her father, she travels to America and is abducted by Indians during the French-Indian Wars and eventually marries one of her captors, a French officer named Philippe de Saint-Christophe (or Christopher).

The film Wrong is Right (1982) starring Sean Connery was loosely based on his novel, The Better Angels.

Novels featuring Paul Christopher or his family

• The Miernik Dossier (1973) Christopher investigates a possible Soviet spy in Geneva
• The Tears of Autumn (1974) Christopher investigates the JFK Assassination
• The Secret Lovers (1977) Christopher discovers a secret plot within the CIA
• The Better Angels (1979) Christopher's cousins steal a Presidential election
• The Last Supper (1983) Introduction to Christopher's parents in pre-WWII Germany; Christopher is imprisoned in China
• The Bride of the Wilderness (1988) Historical novel concerning 17th century Christopher ancestors
• Second Sight (1991) Released from a Chinese prison, Christopher meets a daughter he didn't know he had
• Shelley's Heart (1995) Sequel to "The Better Angels:" Christopher's cousins cause a Presidential impeachment
• Old Boys (2004) Christopher's old associates discover a plot involving terrorists and the fate of Christopher's mother
• Christopher's Ghosts (2007) The story of Christopher's first love in pre-WWII Germany

Non-Christopher family novel

• Lucky Bastard (1999) A comic novel in which a likable but amoral, devious and oversexed politician (meant to invoke Bill Clinton) is controlled by a female eastern-bloc subversive.

Non-Fiction

• Citizen Nader (1972)
• Double Eagle: Ben Abruzzo, Maxie Anderson, Larry Newman (1979)
• The Great Southwest (1980)
• Isles of the Caribbean (National Geographic Society, Washington, DC, 1980, co-author)
• Paths of Resistance: The Art and Craft of the Political Novel (1989, with Isabel Allende, Marge Piercy, Robert Stone and Gore Vidal)
• Inner Circles: How America Changed the World: a Memoir (1992, by Alexander Haig with Charles McCarry)
• From the Field: A Collection of Writings from National Geographic (1997, editor)