She was Altea Town Councillor for urban planning, agriculture, health and public participation (Altea Town Council).In September 2013 she joined the political association ‘Movimiento Ciudadanos’, which is the association which gave rise to the national spread of the political party ‘Ciudadanos’.
In the 2014 European elections, Carolina Punset won the primary elections and third place on the party lists.
In February 2016 she succeeded Juan Carlos Girauta, who is now Ciudadanos’ spokesperson in the lower house of the Spanish Parliament; as Member of the European Parliament (MEP).
Prior to that, Carolina Punset was a Member of the Valencian Regional Parliament and autonomous community spokesperson for ‘Ciudadanos’, a post she had held since the municipal and autonomous community elections in May 2015, having won the party’s primary.
Punset was a member of the National Executive of ‘Ciudadanos’, responsible for the environmental agenda.
In 2012, she stood as an independent Europe Écologie Les Verts candidate in the 5th constituency (French citizens resident in Spain, Portugal, Andorra and Monaco) in France’s legislative elections.
On 20 October 2018 she announced she was leaving 'Ciudadanos', criticising the leadership and citing a shift in the direction of the party.