The pair pledged allegiance to Daesh and its leader Abu Bakr al-Baghdadi, the ministry said in a statement, using an alternative name for the Islamic State group.
They also “launched death threats in the name of Daesh against Spain and France, as well as against other religious groups.”
The suspects are of Moroccan nationality and lived in Spain legally, the ministry said. The man, 32, was arrested in the northern city of Mataro and the young woman, 19, on one of Spain's Canary Islands off the coast of Africa.
The suspects allegedly helped in recruitment, indoctrination and enrollment of new recruits, were in “constant contact with active members in Syria” and distributed multimedia material to teach new recruits how to use arms and explosives.
Like other European nations, Spain has been grappling with a growing number of jihadist cells on its territory and radicalized Muslims leaving to fight for Isis or other Islamist groups in Iraq and Syria. This operation brings the number of suspected jihadists arrested since the beginning of the year to 100, the ministry said.
Spain raised its terror alert to four on a scale of five on June 26th following deadly attacks in France, Tunisia and Kuwait.