On 5 March 2014, Guardado made his 100th appearance for Mexico in a friendly with Nigeria. Selected by Miguel Herrera for the 2014 World Cup in Brazil, he started all the games as a left midfielder, and scored in the last group phase fixture against Croatia, a 3–1 win; they faced the Netherlands in the round of 16, being controversially eliminated after succumbing to a 2–1 defeat. Following the end of the tournament, the manager declared the player would captain the following September friendlies with Chile and Bolivia, in instances when actual captain Rafael Márquez was absent.