Their song "I Need You to Love Me" was released at the end of 2005. The single broke the record on Christian Radio & Retail Weekly's (CRW) Christian CHR chart by holding the #1 spot for 13 consecutive weeks. BarlowGirl was the second most played artist CHR artist of 2005 behind Sanctus Real. It was the most played song on Christian Hit Radio in 2006. BarlowGirl was voted the January 2006 winner in Yahoo!'s Who's Next after viewers were shown the video for the song. BarlowGirl is also among the 12 artists selected to be a part of the first volume of the Big Shiny Planet [UP] Bible Study released nationwide through LifeWay and Family Christian Stores on 2007. The three sisters were youth ambassadors for the National Day of Prayer in 2007.

The Barlow girls' father, Vince Barlow, created youth CDs at his church, Willow Creek Community Church in South Barrington, Illinois. He was hired to perform at events all over the United States. He brought his daughters as his backup band in the late 1990s. BarlowGirl began writing songs and performing them at his performances. The trio stopped touring with their father when Becca and Alyssa began college, but they did perform at his nearby concerts. The trio had written around ten songs by 2002.

The Barlow sisters were given a paid trip to the Gospel Music Association's Music in the Rockies seminar at Estes Park, Colorado, in mid-2002. The sisters were not informed that the seminar was a record industry event for unsigned artists, nor that it was a competition. They reached the finals of the event. Record companies became interested in the sisters after word of mouth spread about the seminar.

The group's name became famous before the group released their first CD. The group Superchic[k] included a song titled "Barlow Girls" on their initial release, Karaoke Superstars, as a tribute to the actual Barlow sisters and their stand for purity, and effectively introduced the sisters to the music world.

The sisters were signed to Fervent Records on October 14, 2003.

BarlowGirl released their first studio album BarlowGirl on February 24, 2004. The album included the longest running number-one song in 2004 on R&R's CHR and CRW's Rock charts, "Never Alone" was named Song of the Year on each of these charts. The CD had sold over 250,000 units by April 2005, and featured the singles "Never Alone" and "Mirror". These number-one songs earned the trio four 2005 Gospel Music Association (GMA) awards (formerly the Dove Award) nominations, including the Best New Artist award, Best Rock Song, and Rock Album. The trio was the best-selling new Christian artist of 2004. BarlowGirl received a 2006 GMA award nomination for Rock/Contemporary Song of the Year for "Mirror". "Never Alone" was also featured on the WOW Hits 2005 CD.

The CD also featured a hidden track titled "Image", which listeners could only find by loading the CD into their computers. To date, it's the second-only track where oldest sister and guitarist Becca sings a solo. She sings the middle part of each verse.

There is also a Family Christian exclusive version which contains the bonus track, "We Pray", which, among others, also features artists Mandisa, Jackson Waters, and Rebecca St. James.

Their second album, Another Journal Entry, was released on September 27, 2005. The album debuted at number three on Soundscan's Christian album chart, and had reached eighty-five on Billboard's Top 200 Current Albums chart by October 10, 2005. The trio was nominated for three additional 2006 GMA awards - "Group of the Year", "Rock/Contemporary Album of the Year", and "Rock Recorded Song of the Year" for "Let Go".

The first single from the album, "Let Go"', was a free download of the week from iTunes. Their next single from the album, "I Need You to Love Me", quickly climbed to number one on the Weekend 22 countdown in April 2006. The single held on to the #1 position on the R&R Christian Hit Radio chart for 9 weeks, and the CRW Christian Hit Radio chart for a record 13 weeks. The single was the most played song of 2006 on Christian Hit Radio as played on the Weekend 22. The band filmed a music video for their hit song "Never Alone" for release on mainstream radio and music video television channels, but it did not chart on the mainstream charts.