Series I consists of two versions of Chisolm's autobiography, written at least twenty-five years after the Civil War. There are two personal notebooks, written around the early to mid 1890s. The first notebook contains genealogical information about the Chisolm and Hazzard families and describes Chisolm's life before the war and his early involvement in the conflict, notably at Fort Sumter and the First Battle of Bull Run. The second notebook documents Chisolm's war experiences from June of 1862 until the end of the war. There is also a version of the autobiography with illustrations that seems to have been intended for publication, written sometime after the death of Chisolm's wife in 1895. His autobiography recounts his childhood in New York, his management of his properties in South Carolina, his wartime services as Beauregard's senior aide-de-camp, and his postwar civilian life. Chisolm describes the battles at Fort Sumter, Blackburn's Ford, the First Battle of Bull Run (Manassas), Battery Wagner, Drewry's Bluff, Shiloh, Petersburg, Franklin, Atlanta, Nashville, the evacuation of Savannah, and the defense of Charleston.

Series II consists of correspondence written during and after the Civil War, mostly by Chisolm and General Beauregard. Much of Chisolm and Beauregard's wartime correspondence is Beauregard's orders to his staff and Chisolm's reports on various battles, though their letters also address an accusation made against Chisolm that he used his official position to obtain transportation on railroads. The postwar correspondence from Beauregard to Chisolm discusses Chisolm's Civil War memorial activities and writings. Other letters written to or authored by Chisolm in the late nineteenth and early twentieth centuries contain Chisolm's remembrances and reflections on the war. There is also some family wartime correspondence, including a letter from Chisolm to his aunt and a letter to A.R. Chisolm from John Chisolm.

Series III consists of documents related to the military created during the course of the Civil War. The series contains a report on the First Battle of Bull Run prepared by Colonel R.G.W. Radford of the 13th Virginia Cavalry (with notes by Chisolm) and general orders issued by the Confederate War Department and by General Beauregard, in which Beauregard officially assumes command of the Military Division of the West. There is also a pass granting Chisolm permission to travel from New Orleans to Richmond, an invitation to a soiree in Charleston extended to various officers, Chislom's notes on aide-de-camps, and a message from Jefferson Davis issued on May 28, 1864 regarding a bill to organize an army staff for the war.

Series IV consists of Chisolm's notes on the war and speeches (both typescript and handwritten drafts) he delivered at various memorial events or before Civil War commemorative groups like the Confederate Veteran Camp of New York and the Survivors' Association of Charleston. His notes and speeches especially focus on the battles at Fort Sumter, the First Battle of Bull Run, and Shiloh. Though Chisolm regretted that his recollections were "obliged to be so personal," he attempted to maintain a neutral tone, citing, for example, the mistakes made by both sides during the Battle of Shiloh. As Beauregard's aide and friend, Chisolm also gave speeches on Beauregard's life and accomplishments following Beauregard's death in 1893. (Researchers should note that Chisolm's "Personal Notes from Before the Surrender of Fort Sumter until the Close of the War" and his speech on the Battle of Shiloh at the Memorial Meeting in Charleston are almost identical, the major variation being that Chisolm's "Personal Notes" contain a preface written months after he delivered the speech.) This series also contains two maps, one of the Shiloh battlefield and one of the Orange and Alexandria Railroad.

Series V is comprised of two scrapbooks which consist mostly of magazine and newspaper clippings or articles pertaining to the Civil War (especially from Charleston's The News and Courier). The loose clippings in this series include articles from The News and Courier regarding Chisolm's lecture on the Battle of Shiloh to benefit the Beauregard Monument Fund, a newspaper clipping about the Confederate Veteran Camp's participation in a memorial service for U.S. Grant, a piece on the reminiscences of a Confederate naval officer, an article by Chisolm in the Confederate Veteran about Beauregard at Shiloh, and various clippings regarding the First Battle of Bull Run. This series also contains a "Roster of the Surviving General Officers of the Confederate States Army" compiled by Telamon Smith Cuyler and a fan-like cipher used by Beauregard for sending messages during the war, with a sample of how the substitution of letters works using the phrase "Jones goes South to night."