Historically, Staffordshire was divided into the five hundreds of Cuttlestone, Offlow, Pirehill, Seisdon, and Totmonslow.

The historic boundaries of Staffordshire cover much of what is now the metropolitan county of West Midlands. An administrative county of Staffordshire was set up in 1889 under the Local Government Act 1888 covering the county except the county boroughs of Wolverhampton, Walsall, and West Bromwich in the south (the area known as the Black Country), and Hanley in the north. The Act also saw the towns of Tamworth (partly in Warwickshire) and Burton upon Trent (partly in Derbyshire) united entirely in Staffordshire.

In 1553 Queen Mary made Lichfield a county separate from the rest of Staffordshire. It remained so until 1888.

Handsworth and Perry Barr became part of the county borough of Birmingham in the early 20th century, and thus associated with Warwickshire. Burton, in the east of the county, became a county borough in 1901, and was followed by Smethwick, another Black Country town in 1907. In 1910 the six towns of the Staffordshire Potteries, including Hanley, became the single county borough of Stoke-on-Trent.

A major reorganisation in the Black Country in 1966, under the recommendation of the Local Government Commission for England led to the creation of an area of contiguous county boroughs. The County Borough of Warley was formed by the merger of the county borough of Smethwick and municipal borough of Rowley Regis with the Worcestershire borough of Oldbury: the resulting county borough was associated with Worcestershire. Meanwhile, the county borough of Dudley, historically a detached part of Worcestershire, expanded and became associated with Staffordshire instead. This reorganisation led to the administrative county of Staffordshire having a thin protrusion passing between the county boroughs (to the east) and Shropshire, to the west, to form a short border with Worcestershire.

Under the Local Government Act 1972, on April 1, 1974 the county boroughs of the Black Country and the Aldridge-Brownhills Urban District of Staffordshire became, along with Birmingham, Solihull, and Coventry and other districts, a new metropolitan county of West Midlands. County boroughs were abolished, with Stoke becoming a non-metropolitan district in Staffordshire, and Burton forming an unparished area in the district of East Staffordshire. On April 1, 1997, under a recommendation of the Banham Commission, Stoke-on-Trent became a unitary authority independent of Staffordshire once more.

In July 2009, the largest hoard of Anglo-Saxon gold ever found in Britain was discovered in a field near Lichfield. The artefacts, known as The Staffordshire Hoard have tentatively been dated to the 7th or 8th centuries, placing the origin of the items in the time of the Kingdom of Mercia.