Smith’s performance with Anderson on 'Midnite Jamboree' brought her a lot of attention. In May 1964, she did some demo recordings, which Anderson's manager, Hubert Long, pitched to 'RCA Victor Records.' Smith's soulful voice impressed the producer, Chet Atkins, who offered her a recording contract. She signed with the label on June 24, 1964.
Under ‘RCA,’ Smith released her debut single, 'Once a Day,' in August that year. The single not only became the greatest hit of her career but also turned into her signature song. Written by Anderson, the song topped the country charts for several weeks, making it one of the few songs in country music history to maintain the first position on the charts for such a long time.
With the historical success of 'Once a Day,' Smith bagged her first three 'Grammy' nominations (for the 'Best Female Country Vocal,' the 'Best New Country and Western Artist,' and the 'Best Country & Western Single'). In March 1965, she released her self-titled debut album, which attained the top position on the ‘Billboard Top Country Albums’ chart for 7 consecutive weeks.
Smith's subsequent albums, 'Cute 'n' Country' (October 1965), 'Born to Sing' (1966), 'Connie in the Country' (February 1967), 'Connie Smith Sings Bill Anderson' (May 1967), and 'Downtown Country' (1967), also ruled the ‘Billboard Top Country’ Albums chart for several weeks.
Around the same time, Anderson wrote several songs for her, most notably, the 'Grammy'-nominated 'Cincinnati, Ohio,' which prompted the city to announce their own "Connie Smith Day" in June 1967. The list also included 'I'll Come Running,' which Smith had written for herself. Anderson also penned the lyrics for the follow-up single to 'Once a Day' (1964), titled 'Then and Only Then.'
In 1965, Smith's childhood dream of becoming a member of the radio show 'Grand Ole Opry' came true. She also performed her hit singles in several country-music vehicle films, such as 'Second Fiddle to a Steel Guitar' (1966), the Jayne Mansfield-starrer 'The Las Vegas Hillbillys,' 'The Road to Nashville' (1967), and 'Hell on Wheels’ (with Marty Robbins).
In 1966, she received a 'Grammy' nomination for 'Connie Smith Sings Great Sacred Songs' and for the single 'Ain't Had No Lovin' from ‘Born to Sing.’ She also bagged a nomination for the ‘Country Music Association’ (CMA) award for the ‘Female Vocalist of the Year’ (1967).
Smith experienced her first career bump in 1968. Her overnight success had brought her extreme pressure from the industry. Added to this were her hectic touring schedules, which affected her mental state, leading her to even contemplate suicide at times. However, her faith in Christianity saved her from taking the drastic step. She became a “Born Again Christian” in the spring of 1968.
On the brighter side, the dark phases of her life not only gave Smith's career a new direction but also taught her to maintain a sound work–life balance. She began to record darker songs, such as 'Ribbon of Darkness' (a cover version of Marty Robbins's hit), which chronicled the traumatic experience of her first divorce. It was nominated for the 'Grammy Award’ for the ‘Best Female Country Vocal.'
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In 1969, she collaborated with country singer Nat Stuckey for the duet album 'Young Love.' Their second album, 'Sunday Morning with Nat Stuckey and Connie Smith' (1970), was a gospel album and was re-released as 'God Will' in 2001. The duo won a 'Grammy' nomination in 1971, for their sacred performance 'Whispering Hope.'
The beginning of the decade saw Smith step into the world of gospel music, which reflected her deepened faith in Christianity. Her next gospel album, 'Come Along and Walk with Me' (1971), is her all-time favorite. She was part of a gospel roadshow with her third husband, evangelist Marshall Haynes.
The year 1972 was the most successful year of the decade for Smith, as all of her singles released that year, 'Just for What I Am,' 'If It Ain't Love,' and 'Love Is the Look You're Looking For,' secured a place among the top 10 songs on the 'Billboard Magazine' chart.
In November 1972, Smith left ‘RCA’ because she felt the label had stopped being courteous to her. The following year, she signed a contract with 'Columbia Records,' under which she predominantly released gospel songs. However, the agreement also allowed her to release country albums. Unlike the country songs, her gospel numbers were relatively less successful. However, that did not have an impact on her stardom, and she remained a top artist for most of the 1970s.
In 1973, she released her first country album, 'A Lady Named Smith' (May), and her first gospel album, 'God Is Abundant' (November). Her gospel performances for 'All the Praises' and 'Connie Smith Sings Hank Williams Gospel' (her second gospel album with 'Columbia') earned her 'Grammy’ nominations.
However, Smith reportedly could not recreate the same quality with 'Columbia' as she had done under 'RCA Victor.' She then signed with 'Monument Records' in 1977. The label prompted her to produce songs that suited the contemporary taste. Hence, Smith shifted her focus to country pop and softer material. She also produced adult contemporary ballads and disco-influenced pop numbers during that phase.
Unfortunately, most of her singles released under 'Monument,' such as her debut album, 'Pure Connie Smith' (1977), could not even secure a place among the top 40 songs of the major charts. Her subsequent singles, 'Smooth Sailin' and 'Ten Thousand and One,' too, failed to appear on any major charts. Smith's only significant hit during that period was the 1977 pop hit ‘I Just Want to Be Your Everything,' which was featured among the top 20 songs on several charts.
The consecutive failures affected the sales figures of 'Monument,' and Smith took a career break in 1979, to focus entirely on her family. That year, she won the 'Music City News Gospel Group/Act of the Year' honor.
Smith made a comeback in 1985, with her new single 'A Far Cry from You,' under 'Epic Records,' which was featured at number 71. Her second single under 'Epic Records,' however, did not enter the charts. She did not release any other studio album in that decade.
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In 1986, she did a cameo in the horror film ‘Maximum Overdrive.'
In 1992, after a gap of several years, she released an album titled 'The Wayward Wind.' An honorary quote by Dolly Parton was included in Smith's 1996 compilation album 'The Essential Connie Smith.'
In 1998, Marty Stuart's label, 'Warner Brothers,' produced her self-titled comeback album. The album, however, was a debacle.
In 2000, Smith reunited a classic country band under the logo of her original band from the 1960s, 'Sundowners,' which was one of the last authentic country bands of the era. She continued to perform in concerts along with the band, and often appeared on the radio show 'Grand Ole Opry.'
In 2002, Smith received one of the highest honors of her career when she attained the ninth position on 'CMT’s list of the “Greatest Women of Country Music.” Another honor came her way when Smith's favorite male country singer, George Jones, mentioned her as his all-time favorite female country singer in his book 'I Lived to Tell It All.'
The following year, Smith released a Christian album, 'Love Never Fails,' in collaboration with Barbara Fairchild and Sharon White (from the country group 'The Whites'). Country singer Martina McBride used a cover version of 'Once a Day' in her 2005 album 'Timeless.'
Continuing as a solo artist, Smith performed Sonny James's hit number 'A World of Our Own' during the ‘Country Music Hall of Fame's “Medallion Ceremony” in May 2007. That year, Smith sang a duet with her husband for his album 'Compadres.'
In November 2008, Smith began making appearances in Stuart's weekly TV series, 'The Marty Stuart Show,' aired on the ‘RFD’ network. After a gap of over a decade, she released a single titled 'Long Line of Heartaches,' under 'Sugar Hill Records.'
Smith was inducted into the 'Country Music Hall of Fame' in 2012.