In 1925, spouses Nathalie Lyons Gray and Bowman Gray Sr., chairman of the R. J. Reynolds Tobacco Company, purchased the 87-acre estate from R. J. Reynolds with the plan of building “the home of their dreams.”[5] The land had formerly been corn fields and pasture for the Reynolda Estate, which is now referred to as the Reynolda Historic District.

[6] The Grays then employed artisans and craftsmen from all over the United States to build what was one of the largest private homes in North Carolina.

[6] At the time, it was second to George Vanderbilt's Biltmore Estate in Asheville, North Carolina, as the largest private home in the state.

[7] Nathalie Gray personally decorated the rooms of Graylyn, and the grounds and gardens were designed by Thomas Warren Sears.

[7] The following day, James R. Scales, the president of Wake Forest University at the time, announced that Graylyn would be rebuilt and restored to its 1932 appearance.