Spanish and Moroccan authorities said they have arrested seven people, including four women and a minor, suspected to be members of an Islamist ring specifically aiming to recruit women for Isis.
Islamic State (Isis) affiliates had set up a recruiting network in Spain to lure local woman into travelling to the Middle East to become jihadi brides, police said.
"The arrested are accused of being part of a network that lured, recruited and sent women to the Syrian-Iraq front for the terror group Daesh [Isis]," Spain's interior ministry said.
Five people were held in separate dawn raids in Ceuta and Melilla, the two Northern African enclaves in Barcelona.
Moroccan police said they arrested the remaining two suspected bride recruiters, in Castillejos, near Ceuta.
Names and personal details of the arrested individuals were not immediately released.
Two of the women were about to leave Spain for the Middle East, Spanish security sources told El Pais newspaper.
The Moroccan Interior Ministry said that, once in Isis-held territories, they were to be used as suicide bombers or married off to a jihadi fighter.
An increasing number of women have joined Isis in Syria and Iraq over the last 12 months, analysts said.
Most have been indoctrinated and radicalised online by recruiters, who usually target young people disillusioned with their lives in the West.
About 100 Spaniards are believed to have joined combat groups in the Middle East, while more than 1,200 Moroccans are reportedly fighting in Syria.