Carroll began his motorsport career in karting in 1993, continuing until 1998. Winning the Elf LA FILIERE SCHOLARSHIP in 1999 led him to British Formula Ford, where he won the Winter Series and finished third in the festival. He raced in British Formula Ford in 2001 before moving to British Formula 3 B-Class in 2002 with the Sweeney team. Despite driving year-old cars, Carroll dominated the class, winning the title with a record points tally.
In 2003, Carroll moved up to Championship Class British Formula 3, but faced financial constraints. He drove for three different teams, achieving eight podiums in a row, and also participated in the Formula Three Euroseries, scoring points in his first race. He outperformed future Formula One driver Nico Rosberg in an end-of-season event in South Korea. Carroll continued in Formula Three throughout 2004, finishing as runner-up to Nelson Piquet Jr., before joining the 2005 GP2 Series with Super Nova Racing. Despite a late deal and limited pre-season testing, he was immediately competitive, briefly challenging for the championship before reliability issues and on-track incidents hampered his progress.
Carroll’s talent attracted the attention of Formula One, and in 2005 he became a test driver for BAR-Honda. For the 2006 GP2 season, he joined Racing Engineering. He achieved a pole position, third place, and second place at Silverstone. He finished eighth in the championship, equal on points with Gianmaria Bruni, and crucially scored all of his team’s points, outscoring his previous team, Super Nova Racing.
In 2007, Carroll drove a two-year-old Audi A4 in the German DTM series. He briefly returned to GP2 with FMS GP2, winning at Silverstone and the Hungaroring feature race. Sponsorship problems led him to leave the DTM and focus on GP2, finishing seventh overall. He also tested the A1GP car for Ireland, leading to a drive in the series. He scored Ireland’s biggest points haul in A1GP history with a podium in his first race, and later won the Mexico City feature race, securing Ireland's first A1GP victory. He helped Team Ireland finish sixth overall in the championship.
Carroll participated in four races for FMS International in the 2008 GP2 Series before being replaced by Marko Asmer. He returned to A1GP with Team Ireland in 2008/2009, leading them to their first championship victory in China. A1 Team Ireland became the fourth A1 Grand Prix champions, winning with 112 points, all scored by Carroll, including five race victories and three fastest laps.
In April 2009, Carroll was approached by Campos Meta and Manor GP regarding a Formula One drive in 2010, but could not raise the necessary funding. A potential drive with Lola also did not materialize when the marque's entry was rejected.
Carroll competed in some races for Andretti Autosport in the IndyCar Series in 2010, finishing sixteenth at Watkins Glen and nineteenth at the Honda Indy 200, scoring a total of 26 points. In 2011, he made a one-off appearance in Formula Renault 3.5, finishing fourth and third, and also drove in Auto GP, taking pole position and finishing fifth and second. He returned to GP2 with Super Nova Racing for the German round onwards, replacing Luca Filippi.
In the 2020–21 Formula E season, Carroll was signed as NIO 333's reserve driver. In 2023, he joined Team WRT in the GT World Challenge Europe Endurance Cup and added a part-time campaign in the GT World Challenge America with Esses Racing.
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