He continued his emergence as a star midfielder in 2012, averaging 22 possessions and earning three Brownlow votes for best-on-ground in crucial wins over Sydney and Fremantle.

[9] Midway through the year, he revealed he had signed a three-year deal with the Crows, saying, "The way Brenton [Sanderson] and the rest of the coaching staff have gone about creating this really enjoyable environment for us to be involved in - I think that's a big reason why everyone wants to stay around".

[9] Due to the season-ending Achilles injury sustained by captain Nathan van Berlo during pre-season training in 2014, Sloane and Patrick Dangerfield were named as acting co-captains of the Adelaide Football Club for the 2014 season.

[12] Sloane twice injured his cheekbone during the season, missing a total of five games, but despite that remained one of the club's elite players, finishing sixth in Adelaide's best and fairest.

He started to struggle when other teams began heavily tagging him, Melbourne notably playing ex-Crow Bernie Vince on him, causing the Crows to lose their next two matches.

[16] Sloane worked hard to improve against these tags, but again he struggled against Melbourne in round 17 when Vince kept him to just 8 possessions before he was knocked out in a Dean Kent tackle and sat out the rest of the game.

[19] Sloane's future was up in the air during the 2018 season as multiple clubs were eager to lure him back to his home state in Victoria, with Collingwood looming as a likely suitor.

In 2020, Sloane assumed the sole captaincy and in round one played his 200th AFL game against the Sydney Swans at the Adelaide Oval,[21] which the Crows lost by three points.

[22] Despite the club's least successful year in their history, Sloane continued to serve as captain during the majority of Adelaide's games and amassed 3 Brownlow votes.

[28] Sloane featured in the 2021 fly-on-the-wall documentary TV series Making Their Mark, which showed the impact of the COVID-19 pandemic on several AFL clubs, players, and staff.

[29][30] Nic Naitanui and Eddie Betts were filmed almost continuously, with other players featured including Stephen Coniglio and Sloane, along with several coaches and other staff associated with the clubs.