After a disappointing finish at the 2004 U.S. Olympic Outdoor Trials, Jones finished second in her first professional meet at Stuttgart. She had a stellar 2006 campaign, which saw her win at Heusden-Zolder in July, running a personal best time of 12.56. At the 2006 World Athletics Final, she finished sixth in the 100m hurdles and fifth in the 100m. She also did well on the European circuit, winning the meet in Ostrava. She finished the 2006 season ranked fourth in the U.S. and seventh in the world by Track & Field News.
Jones won her first national championship in 2007, winning the 60m hurdles at the USA Indoor Championships with a time of 7.88 seconds. In the European winter circuit, Jones won two meets and finished second in two others in the 60m hurdles. In April, She won the 100 meter hurdles at the Drake Relays. At the 2007 USA Outdoor Track and Field Championships, Jones finished third in the 100m hurdles, thereby earning a spot on the U.S. Team at the world Championships in Osaka, Japan, where she finished 6th. On the summer track circuit, Jones won meets at Rethimno and Heusden along with second-place finishes at Doha, Sheffield, and Monaco.
Jones started the 2008 season with hopes of making the 2008 summer Olympics. She began the indoor campaign with second place finishes in Glasgow, Gothenburg, and Stuttgart in the 60m hurdles. she then picked up a win in Dusseldorf, setting a meet-record in the process. In Karlsruhe, Jones ran a personal best time of 7.77 seconds and finished second to Susanna Kallur, who broke the world record with a time of 7.68 seconds. Jones' time was the second-fastest ever by an American. She was named USA Track & Field's Athlete of the Week on February 12 for her performance in Karlsruhe. At the 2008 USA Indoor Championships, Jones won her second straight national championship with a time of 7.88 seconds and also won the Visa Championship Series title for the 2008 indoor season. At the World Indoor Championships in Valencia, Spain, Jones won the 60m hurdles with a time of 7.80 for her first world championship.
Jones opened the 2008 outdoor season with a first place finish at the LSU Alumni Gold meet in Baton Rouge, setting a stadium record in the process.
At the 2008 Beijing Olympics, Jones went into the 100m hurdles final as a favorite, and was comfortably in the lead coming into the final stages. However, She clipped the 9th of 10 hurdles, breaking her stride and momentum and finished the race in 7th. Comparisons were made between Jones and Gail Devers, who came into the 1992 Barcelona Olympics as the heavy favorite in the 100m hurdles, only to stumble on the 10th hurdle and thus not placing. American Dawn Harper ended up taking a surprising gold in 12.54 seconds.