According to an Interior Ministry report, the Spanish woman had returned to Spain through Málaga airport after having stayed with family in Turkey, from where she hoped to travel to Syria.
The 26-year-old woman reportedly left Spain about a year ago with her partner with the intent to join Isis in Syria. She had gone with the rest of her family to Turkey and lived in a region along the Turkish-Syrian border where Isis is said to have a strong presence.
A video released by the ministry and the National Police shows the woman being led by security forces off of a Turkish Airlines plane with its engines running on the tarmac. The woman's face is covered with a scarf as she is shown to a police vehicle.
The woman is being transferred to police headquarters in Madrid.
Earlier this week, authorities said they had arrested three Moroccans who allegedly had links to Isis and were planning terror attacks in Spain and also detained two men suspected of recruiting for the jihadist group in Catalonia.
The arrest also comes just weeks after a 22-year-old Spanish "good Catholic girl" was arrested in Madrid airport, allegedly on her way to join Isis, travelling through Turkey.
A growing number of jihadist cells have emerged on European soil, with members leaving to fight for Isis or joining rebel fighters in Iraq and Syria.
More than 100 people from Spain are reported to have left to join jihadist fighters and officials are afraid they may return to plan attacks.