Angier is a town in the Black River Township of Harnett County, North Carolina, United States. The population was 4,350 at the 2010 census and estimated as of 2016 to be 5,096. Angier is a part of the Dunn Micropolitan Area, which is also a part of the greater Raleigh?Durham?Cary Combined Statistical Area as defined by the United States Census Bureau.