Toye and Colm McFadden were in the same class at primary school; they played in the Ted Webb under-16 tournament, the same year they were part of the county minor team. Toye burst onto the national scene with goals in the Championship against Meath in 2002 and Armagh in 2003, both at Croke Park. He played for Donegal against Armagh in the 2004 Ulster Senior Football Championship Final at Croke Park, but went off injured and was replaced by Rory Kavanagh. He captained Donegal in the 2006 Ulster Senior Football Championship Final against the same opponents at the same venue. He was a member of the Donegal team that won the NationalFootball League in 2007, playing from the start to the end in the final against Mayo. In 2009, while in the form of his life, Toye ruptured his Achilles tendon during an All-Ireland qualifier against Clare at MacCumhaill Park. He was left as a spectator when Armagh knocked Donegal from the 2010 Championship in Crossmaglen. However, Toye returned the following season, rejuvenated by the arrival of Jim McGuinness as manager. He did not feature in the NFL or Ulster campaign but was sprung from the bench in the 2011 All-Ireland quarter-final against Kildare at Croke Park. Within 25 seconds of his first appearance in 25 months he had the ball in the back of the Kildare net, later making a further vital contribution by scoring the final equalising point of a game which Donegal went on to narrowly win through a memorable point from Kevin Cassidy in extra-time. Toye had previously scored a goal for Donegal at Croke Park in a 2003 All-Ireland semi-final. Indeed, with four goals, Toye is Donegal's record goalscorer at Croke Park — one goal each against Meath, Armagh, Cork, and Kildare. He came on as a second-half substitute for Leo McLoone in the 2012 All-Ireland Senior Football Championship Final, won by Donegal. He missed the entire 2013 season while battling trigeminal neuralgia but was back in 2014 in time for another shot at the All-Ireland. On 20 September 2014, he was named to start against Kerry in the following day's All-Ireland Final. In January 2017, Toye retired from the inter-county game.
Club
Toye's club have not had much success at senior level. They reached the final of the 2011 Donegal Senior Football Championship— their first ever senior final—but lost, though Toye scored three points. Previously, in 2004, they reached the final of All-Ireland Intermediate Club Football Championship, in which Toye scored a point.
Other work
Toye has been active in encouraging people to read more books.
Honours
;Donegal
All-Ireland Senior Football Championship: 2012
Ulster Senior Football Championship: 2011, 2012, 2014
National Football League Division 1: 2007
;Naomh Mícheál
All-Ireland Intermediate Club Football Championship runner-up: 2004
Ulster Intermediate Club Football Championship: 2003
