The 2004 season was a significant breakthrough for Moore, starting with a 100 m personal record of 11.26 seconds at the SEC Championships. Later that year she a 200 m best of 22.63 seconds in the semi-finals of the NCAA Women's Outdoor Track and Field Championship before going on to win the final in a wind-assisted 22.37 seconds. She was also fourth in the 100 m in 11.31 seconds. In July she took third in the women's 200 m at the 2004 United States Olympic Trials behind Allyson Felix and Muna Lee, gaining her qualification in the event for the 2004 Summer Olympic Games. She reached the Olympic semi-finals of the women's 200 m but could not match her form of earlier in the season, finishing sixth in a time of 22.93 seconds. Her following two seasons were low profile, with 2005 being highlighted by a 100 m win in Salamanca, and 2006 performances in the 200 m including a win at the Reebok Grand Prix and a fifth-place finish at the USA Track and Field Championships. She began training with Olympic gold medalistJon Drummond during this period. Her Olympic year form returned in 2007, which she began with personal record-equalling run of 11.26 seconds at the Mt. SAC Relays and an outright 200 m best of 22.46 seconds to finish as runner-up at the Adidas Track Classic. She finished fourth in the 200 m at the 2007 US Outdoor National Championships, but due to the fact that the race winner was automatically qualified for the 2007 World Championships in Athletics as the reigning world champion, Moore gained a position on the US team. She went on to be one of four American women to reach the 2007 World 200 m final but she only managed seventh place with a below-peak form run of 22.97 seconds. After making appearances in the 2007 IAAF Golden League, at the ISTAF and Memorial van Damme meetings, she closed the season by winning a bronze medal at the 2007 IAAF World Athletics Final – her first global senior medal.
2008–2010
Moore's 2008 season peaked at the Olympic Trials, where she recorded a 100 m best of 11.03 seconds in the qualifiers but was eighth in the final with 11.22 seconds. She was knocked out of the 200 m trials at the semi-final stages and did not compete at the 2008 Olympic Games. The following year she reached the 200 m final at the 2009 US National finals, but finished in last place and missed out on qualification for the 2009 World Championships in Athletics. She had a strong start to the 2010 outdoor season in April, running an early world lead and 100 m meet record of 11.06 seconds at the Drake Relays. She equalled her 200 m best in Baie Mahault in May and went on to win the 100 m at the Grande Prêmio Caixa Maringá de Atletismo in Maringá, Brazil later that month, going sub-11 for the first time in a personal best run of 10.97 seconds. It was the first time any female had broken the 11 second barrier on South American soil. She took second place in the 100 m 2010 USA Outdoor Track and Field Championships, finishing behind Allyson Felix.