In 2009, Pooley signed to the Cervélo Test Team, where she remained until their disbandment at the end of 2011. She won the 2009 national time trial championships and took wins for the team in the Coupe du Monde de Montreal, GP de Plouay, and Grand Prix Costa Etrusca one-day races, and the final edition of the Grande Boucle Féminine, once dubbed "the women's Tour de France". Due to financial issues the 2009 Grande Boucle was reduced to only four stages, leading Pooley to joke that it was "more of a Petite Boucle than Grande". She also wore the leader's jersey for three stages of the Giro d'Italia Femminile, but finished the race in fourth place in the general classification after losing the race lead due to her poor descending, which she improved after the 2009 season with the help of her coach Tim Williams and British Cycling psychiatrist Steve Peters.
