[2] In 1973, Ayoub became a founding member of the Polisario Front (PF), which aimed to free Western Sahara from Spanish and Moroccan rule.
He was close with El-Ouali Mustapha Sayed, who would later become President of the Sahrawi Arab Democratic Republic, and sat on PF's executive committee from 1976 to 1989.
Following El-Ouali's death, he travelled to Nouadhibou on 6 June 1976 and attempted to assassinate President of Mauritania Moktar Ould Daddah.
In May 1977, he led Polisarian forces in the Battle of Zouérat [fr] and attacked several hundred French aid workers and their families.
In October 1981, he commanded the Battle of Guelta Zemmur, where Polisarian anti-aircraft units shot down a C-130, a Mirage F1, a Northrop F-5, and a helicopter, all belonging to Morocco.