Wynne is the largest city in and the county seat of Cross County, Arkansas, United States. The population was 8,314 at the 2020 Cens…Wynne is the largest city in and the county seat of Cross County, Arkansas, United States. The population was 8,314 at the 2020 Census. Nestled between the Arkansas Delta and Crowley's Ridge, Wynne is the closest city to the second-largest state park in Arkansas, Village Creek State Park.