NC 241 has existed twice before. The first existed for one year, from 1923 to 1924; it traveled from NC 60, in Jonesboro, to NC 24, in Fayetteville. It was replaced by an extension of NC 53.
The second NC 241 was established in 1930 as a new primary routing, from NC 70, in Aberdeen, south through Laurinburg, to the community of Johns. In 1931, it was extended south to NC 130, in Seven Bridges. In 1932, NC 241 was straightened out between Laurinburg and Aberdeen; the same year, US 311 was assigned to the entire routing of NC 241. In 1934, US 501 replaced US 311 along the route and also decommissioned all of NC 241.
The third and current NC 241 was established in 1971, as an upgrading of secondary roads SR 1005, in Duplin County, and SR 1106, in Lenoir County.