Laybourne was born Geraldine Bond on May 19, 1947 in Martinsville, New Jersey, a rural community of about 400. She is the second of four children, born to a former radio writer/actress and community organizer and a stock broker.

Laybourne built Nickelodeon into the first global television network to profit from selling advertising targeted towards children. Her programming approach, which made a point of talking to children as equals, built the tiny cable network, which had only five employees in 1980, into an $8 billion Business.

Laybourne was one of the first people to focus on television programming for kids. She spent 15 years at Nickelodeon, taking over the management of the network, and started accepting advertising for the network, in 1984.

In 1996 Laybourne was ranked No. 1 among the 50 Most Influential Women in the Entertainment Industry by The Hollywood Reporter and named one of the 25 Most Influential people in America by Time Magazine. She has been awarded the Annenberg Public Policy Center’s award for Distinguished Lifetime Contribution to Children and Television, the New York Women in Communications Matrix Award for Broadcasting, the Creative Coalition’s Spotlight Award, the Grand Tam Award from the Cable and Telecommunications Association for Marketing (CTAM), the Governor’s Award from the National Academy of Cable Programming, the Alliance for Women in Media Genii Award, the Women in Cable Award, the Sara Lee Corporation’s Frontrunner Award, the Entrepreneur of the Year Award from the University of Missouri–Kansas City and the New York Women in Film & Television Muse Award.

Laybourne has been on the Board of Vassar College (since 1998). She is an advisor to Springboard, Vital Voices and Acumen Fund. Laybourne sat on the boards or advisory committees of The National Cable & Telecommunications Association, The National Council for Families and Television, New York Women in Film & Television (Advisory Board), and Cable Positive (Honorary Chair), and The White House Project.

On February 2, 2000 (a date which plays off the chemical compound of oxygen—O2/O2), the Oxygen Network premiered to 10 million subscribers.

LVMH was an early investor, but left in 2001 when Laybourne changed strategy from being an Internet company to a television company.

Laybourne initially hired 700 people, but scaled down to 250. The company went on to become profitable in 2004. Microsoft Billionaire, Paul Allen, who invested in three rounds of Oxygen, forced Oxygen's sale in the late 2007 to NBC Universal for $925 million. At the end of Laybourne's tenure, Oxygen had 270,000 prime-time weekday viewers in 74 million homes.

Laybourne was inducted into the Broadcasting & Cable Hall of Fame, Cable Center Hall of Fame, and the Advertising Hall of Fame. She was inducted into She Made It, an initiative of the Paley Center in 2005. She is a member of the cable industry's Entrepreneurs Club.