On 29 September 2010, Ablett signed a five-year contract valued at $9 million with the Gold Coast Football Club, a side entering the AFL for the first time in 2011. On 19 January 2011, after much speculation, Ablett was named the inaugural captain of the Suns. In the club's inaugural season, Gold Coast finished last on the ladder with a 3–19 win-loss record, meaning that Ablett missed out on playing in a final for the first time in five years; he still had a great individual season, finishing with career-highs in tackles (119) and clearances (133) and being named captain in the 2011 All-Australian team. In 2012, Ablett continued his individual success, winning his fourth Leigh Matthews Trophy and finishing the season with a career-high in kicks (389). In 2013, Ablett had a tremendous season, leading the league in average disposals (31.2) and taking home his second consecutive (and fifth overall) Leigh Matthews Trophy. He also won his second Brownlow Medal, becoming the first Gold Coast player to win the award and the 14th player in VFL/AFL history to win it twice. Ablett became the fifth player to win Brownlow Medals at different clubs, joining Ian Stewart, Peter Moore, Greg Williams and Chris Judd. Ablett had a career-best season in 2014, averaging 32 possessions and kicking 24 goals before suffering a season-ending shoulder injury in the Sun's win against Collingwood in round 16. Despite playing only 15 games, he finished equal-third in the Brownlow Medal with 22 votes.