George F. Round was born on January 5, 1840 in Newton County, Georgia. He was the eldest son of Methodist minister George Hopkins Round and his wife, Mary Louisa McCants Round. Round grew up in Cokesburg, South Carolina. He entered Dickinson College in Carlisle, Pennsylvania as a member of the class of 1861. His brother, William Capers Round, joined him in the class of 1863. While at the College, George Round was elected to the Belles Lettres Society and became a member of Phi Kappa Psi. He did not finish his degree, however, for he withdrew from Dickinson and returned home when the war began.
Round enlisted in Company K (Spartan Rifles) of the Fifth South Carolina Volunteer Infantry in Spartanburg, South Carolina. How much fighting he saw personally is unclear, but the Fifth South Carolina was in action in some of the fiercest fighting of the war. They were in A.P. Hill's Division, then in Longstreet's, and at Gettysburg served as a part of Pickett's Division. The Fifth South Carolina ended the war at Appomattox Court House as a part of Bratton's Division. Round's brother William did not survive the conflict.
Following the war, Round returned to his studies, this time at Wofford College in Spartanburg, South Carolina. After graduation, he entered the Methodist ministry under the South Carolina Conference, serving in Anderson County in his early years. Round was a pastor in Caldwell County, North Carolina for a time and then, in 1885, went west to Oregon and served at Newbern in Yamhill County. He spent the rest of his life in the state and affiliated with the Oregon Conference in 1888.
In March 1867, while in Anderson County, Round married local girl Julia Hammond. The couple had five children, three boys and two girls. Around 1880, Julia died and Round married Louisa Painter, a woman of his age and a native of Caldwell County. They had no children. George F. Round died in Canyon City, Oregon on May 2, 1928. He was eighty-eight years old.