Downtown Country was a departure from Smith's previous albums, as most of the material was more Pop-oriented and featured cover versions of Pop music material as well. Violins, violas, and other orchestral arrangements were incorporated into the album's material to add a more Pop-sounding style. The album consisted of twelve tracks, many of which were cover versions, including Petula Clark's "Downtown," Elvis Presley's "It's Now or Never," Sandy Posey's "Born a Woman," Lynn Anderson's "Ride, Ride, Ride," and Connie Francis's "My Heart Has a Mind of Its Own." The album was released on a 12-inch vinyl LP record with six songs on each side of the record, and was recorded in Nashville, Tennessee. Reviewed by Allmusic, Downtown Country was a given a rating of four out of five stars.
Downtown Country spawned only one single, the Harlan Howard-penned, "The Hurtin's All Over." Released in September 1966, the song became a major country hit, peaking within the Top 5, reaching #3 on the Billboard MagazineHot Country Songs chart in early 1967. In addition, the album itself also reached a peak position. Downtown Country reached a peak of #5 on Billboard's Top Country Albums chart, becoming Smith's last Top 5 album. It was Smith's first album to be released in 1967 as well.