Assigned to duties in the vicinity of Brandy Station until early May 1864, the 72nd New York assisted with operations along the Rapidan River (February 6–7), and was then assigned to the Overland Campaign led by Lieutenant-General Ulysses S. Grant. After fighting in the battles of the Wilderness (May 5–7), Spotsylvania Court House (May 8–21), North Anna (May 23–26), Totopotomoy Creek (May 28–31), and Cold Harbor (June 1–12), the regiment also participated in the opening weeks of the Siege of Petersburg until its leaders received orders to begin winding down the regiment's operations. On June 20, Companies A, B, D, E, F, I and K mustered out. Companies C, G, and H were then transferred to the 120th New York Infantry. Company G was then officially mustered out on July 2, followed by Company C on July 20 and Company H on October 31, 1864.