The Barlow sisters' father, Vince Barlow, created youth CDs at his church. 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 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.

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".

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.

The members of BarlowGirl were the youth ambassadors for the National Day of Prayer in 2007. They recorded the song "We Pray" for the event, along with other artists such as Rebecca St. James

BarlowGirl recorded with producer Otto Price for their third studio album How Can We Be Silent. The album was released on July 24, 2007. How Can We Be Silent debuted at #1 on Billboard's Christian Chart, and #40 on Billboard's Top 200 albums. The first single from the album, "Here's My Life", was released in June 2007. Their second single, "Million Voices", was released to rock radio a few weeks later. The third single, "I Believe In Love", was released on October 8, 2007.