The village was established as "Centreville" on October 4, 1815, by Peter Bohart, owing to its location at the crossroads of the routes between Steubenville to Canton and New Lisbon to New Philadelphia.

[6] The village derives its name from Charles Carroll of Carrollton, the last surviving signer of the Declaration of Independence.

[7] Many of the Fighting McCooks of Civil War fame lived in Carrollton.

The Daniel McCook House is listed as a National Historic Place.

[8] According to the United States Census Bureau, the village has a total area of 2.45 square miles (6.35 km2), all land.

A branch of the Wheeling and Lake Erie Railway passes through and ends at the Carroll County Industrial Park.

As of the census[12] of 2010, there were 3,241 people, 1,347 households, and 829 families living in the village.

The village's population was spread out, with 21.4% under 18, 8.1% from 18 to 24, 24.0% from 25 to 44, 23.4% from 45 to 64, and 23.0% who were 65 years of age or older.