Smith's earliest broadcasting job was for Metromedia Television, where he served as White House correspondent for WTTG. Metromedia would later transfer him to New York, where he would become co-anchor of WNEW-TV's 10 PM newscast.
Smith departed Metromedia for CBS in 1970, and instantly became a reporter and anchor for WCBS. In 1973 Smith was named co-anchor of WCBS' evening newscasts, a position he held for 13 years. His 11 PM co-anchors included Dave Marash (1973–1978 and 1981–1982) and Vic Miles (1978–1979), before Michele Marsh joined him for the balance of his run with channel 2. Starting in late 1975, he was teamed with Jim Jensen on the 6 PM newscast, a partnership that remained until Smith's departure from the station.
He left WCBS when he was promoted to co-host of CBS' The Morning Program in January 1987. Smith left CBS that December after the show was canceled. Following this he moved to WWOR, and in early 1988 he became the lead anchor of the station's 10 PM newscast replacing Tom Dunn. Smith would leave WWOR in 1993 and moved from New York for the first time since his transfer from Washington, as he relocated to San Diego to take an anchor position at NBC affiliate KNSD. This was the first time Smith had worked for a network-affiliated station since his 1987 departure from WCBS (WWOR, at the time, was an independent and was a year away from gaining any affiliation). He stayed with KNSD until 1997 and returned to New York, but did not immediately return to television.
After a four-year absence (which included a brief stint at WRNN), Smith rejoined WWOR as lead anchor following Ernie Anastos' departure to return to WCBS. He eventually moved to weekends as the co-anchor of the station's now-former Saturday and Sunday newscasts. In addition to his anchor duties, on each newscast he provided a small commentary that would be accompanied by his signature superimposed on screen. After a long career Smith announced his retirement in 2006, ending a nearly 40-year career with 11 Emmy Awards for his body of work.
Outside of news
In addition to his news career, Smith is a published poet with several books and CDs of his writings in print. As a part of WWOR during its time being owned by MCA, he made a cameo appearance in the now-extinct King Kong Encounter at Universal Studios Hollywood.
"Fighting the frizzies, at 11"
This obscure-in-origin catchphrase among both Star Wars and South Park fans traces its origins to Rolland Smith. Star Wars Holiday Special is commercially unavailable except for the bootleg copies of home VHS and Betamax recordings of the show's one-time airing. Among the most widely circulated recordings is one made from the broadcast on WCBS-TV, though recordings of the broadcast from many other CBS affiliates as well as overseas broadcasters abound.
During the WCBS broadcast, a young mustachioed Smith appears during a number of commercial breaks in a "teaser" for the upcoming 11 PM newscast, where he simply says "Fighting the frizzies, at 11", probably in reference to a story on hair care. The creators of South Park, Matt Stone and Trey Parker - both huge fans of the Star Wars special - incorporated scenes of South Park editor Tom Vogt dressed as a news anchor resembling Smith in a South Park holiday episode. The episode opened with the line being deadpanned by Vogt, and each segment of the show began with the line (or some variation of it). The episode ended with the anchor fighting a hairy creature.