After successfully co-chairing a campaign to elect Elizabeth May as Leader of the Green Party of Canada, Carr resigned her position of Leader of the Green Party of British Columbia in September 2006 to become one of two deputy leaders of the Green Party of Canada appointed by her political ally and long-time friend Elizabeth May. In January 2007, Carr was nominated to run in the federal riding of Vancouver Centre, running against Liberal Party of Canada incumbent Hedy Fry. That same year Carr bought a condominium in the West End and succeeded in getting the party to open up a regional office in BC at the Dominion Building, 301-207 West Hastings Street within the riding (February 2007)(relocated to suite 403 in the same building in December 2011). Her work for the federal party serving as the co-chair of the party's Shadow Cabinet, member of the national Campaign Committee and chair of the national Fundraising Committee