Buckleboo began as a government town, surveyed in November 1924 and proclaimed on 17 December 1925 by Tom Bridges, the Governor of South Australia. It was named after the cadastral unit of the Hundred of Buckleboo. On 27 July 1989, the extent of the government town was reduced by the removal of land north-west of Myrtle Street. Boundaries for the locality were established in 1999, encompassing the government town of Buckleboo and the former government town of Moongi. In 2013, a parcel of land was removed from the adjoining locality of Pinkawillinie and added to Buckleboo to ensure that the area once covered by the Buckleboo Pastoral Run was within the locality.
Until 2005, Buckleboo was the railhead for one branch of the Eyre Peninsula Railway, a narrow-gauge railway that principally hauled grain via Kimba and Cummins to Port Lincoln for export. The silos at the former railway station and the few remaining buildings are surrounded by the Buckleboo Conservation Reserve, proclaimed in 1990.
Maintance plan has been submitted