It is bordered by the provinces of Madrid, Cuenca, Ciudad Real, Badajoz, Cáceres, and Ávila.
Of the province's 546,538 people (2002), only about 1/9 live in the capital, Toledo, which is also capital of the autonomous community.
The province contains 204 municipalities. The smallest municipality in Spain, Illán de Vacas, with a population of 5, is in Toledo province. See List of municipalities in Toledo.
The province shares the Parque Nacional de Cabañeros with Ciudad Real province.