McCool first came to World Wrestling Entertainment (WWE) as a competitor in the 2004 WWE Diva Search, losing to Christy Hemme. Although she was eliminated, WWE signed her to a three year deal in November. Despite not winning the contest, she later debuted on SmackDown! as a fan favorite with a "Personal Trainer" gimmick.She wrestled in her first SmackDown! match, teaming with The Big Show to defeat Dawn Marie and René Duprée on March 3, 2005. A few months later, McCool became a part of the feud between MNM and Heidenreich when she defended Heidenreich against MNM's manager Melina's verbal attacks. In a match on June 30, Melina defeated McCool by pinning her with the illegal aid of the ring ropes as leverage. After the match, MNM performed their finisher, the Snapshot, on McCool.
McCool was then sent to WWE's developmental facility, Deep South Wrestling (DSW), where she wrestled, performed interviews, hosted segments, and provided color commentary. While in DSW, she was hospitalized after having an allergic reaction to a prescribed medication and was temporarily sidelined to recover. Eventually, she started to train in WWE's other developmental territory, Ohio Valley Wrestling (OVW). While in OVW, she began managing the duo of Amish Roadkill and K.C. James.
She returned to SmackDown! on June 2, 2006, this time working as a villainous character with a "sexy teacher" gimmick, pulling on her real life experiences. Upon her arrival, she aligned with Kristal Marshall to feud with Jillian Hall and Ashley Massaro. This feud led to a Fatal Four-Way Bra and Panties match at The Great American Bash, which Massaro won. She won her first singles match on the July 28 edition of SmackDown!, defeating Hall by illegally using the ropes as leverage. Soon after, she began acting as valet for the team of K. C. James and Idol Stevens, who, because of her association with them, were nicknamed The Teacher's Pets. The trio began feuding
with Paul London and Brian Kendrick, and their valet Massaro, for the WWE Tag Team Championship, but never won the title. The feud ended when London and Kendrick won a match against them at No Mercy in October. On November 28, McCool was hospitalized with an enlarged kidney, a broken sternum, and an electrolyte imbalance. She was released from the hospital on December 2.
McCool returned on the March 30, 2007 edition of SmackDown!, where she participated in a 10-Diva tag team match. On the April 13 edition of SmackDown!, McCool became fan favorite once again when she came to the aid of Ashley Massaro after she was attacked by Jillian Hall backstage. On the May 28 edition of Raw, McCool won the Memorial Day Bikini Beach Splash Battle Royal by eliminating Melina. Subsequently, a series of matches took place between Victoria and McCool, including a Mixed Tag Team match where Victoria and Kenny Dykstra defeated McCool and Chuck Palumbo.
McCool then became caught in the middle of a feud between the villainous Jamie Noble and her on-screen friend Chuck Palumbo. After a series of matches between the men, Noble won a date with McCool by defeating Palumbo in a match. In the storyline, Palumbo accidentally elbowed McCool during a match, causing her to suffer a concussion. The partnership was dissolved when McCool refused to accept his apology. She then went on to compete in a series of contests with Victoria, Eve Torres, Maryse and Cherry to determine SmackDown!'s top Diva, subsequently winning the title. At The Great American Bash on July 20, 2008, McCool defeated Natalya Neidhart to become the inaugural WWE Divas Champion.
On the December 26, 2008 episode of SmackDown!, McCool lost the WWE Divas Championship to Maryse. After the match McCool blamed Maria, the special guest referee of the match, for her loss and attacked her, establishing herself as a heel. In the following weeks, McCool also attacked Eve Torres, resulting in Eve's debut match, which McCool won. McCool then defeated Gail Kim on the May 22 taping of SmackDown to become the number one contender for the WWE Women's Championship, which she would win a month later at The Bash by defeating Melina. She retained the championship against Melina during a rematch on July 26 at Night of Champions.
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McCool then formed an alliance with Layla, and entered into a feud with Mickie James, which resulted in a five-on-five Elimination match at Survivor Series, which James' team won. James then became the number one contender for McCool's championship at TLC: Tables, Ladders & Chairs, where McCool successfully retained the championship. However, McCool lost the WWE Women's Championship to James at the 2010 Royal Rumble, though she regained it on the February 26 edition of SmackDown when special guest referee Vickie Guerrero interfered, costing James the Championship. On the April 23 edition of SmackDown, she and Layla attacked Beth Phoenix with a spray and table. The attack was a reference to the upcoming Extreme Makeover WWE Women's Championship match between McCool and Phoenix at the 2010 Extreme Rules, which McCool lost. On May 14, 2010, McCool and Layla faced the then-WWE Women's Champion Phoenix in a two–on–one handicap match, in which Layla pinned Phoenix and won the WWE Women's Championship.
On the July 20 edition of SmackDown, McCool took the place of Layla in her WWE Women's Championship match against Tiffany, defeating her and retaining the title. At Night of Champions McCool defeated Melina to unify the WWE Women's Championship and the WWE Divas Championship, thus becoming the first ever WWE Unified Divas Champion. At Survivor Series on November 21, she lost the Divas Championship when Natalya defeated McCool and Layla in a two-on-one handicap match. At TLC: Tables, Ladders and Chairs, she and Layla were defeated in the first ever Divas tag team tables match by Natalya and Beth Phoenix.