According to a police statement, the arrests were made on Wednesday as part of an operation which included 13 raids in the Barcelona and Tarragona areas.
The statement added that some 360 Mossos d'Esquadra regional police officers participated in the huge offensive, which was coordinated by the National Court in Madrid.
Authorities have so far busted a number of recruitment cells in Spain, including in the country’s North African territories of Ceuta and Melilla.
Earlier this month, four members of a family, including 16-year-old twin boys, were arrested in Catalonia for seeking to join the ranks of Takfiri militant groups in Syria.
Eight suspected members of a Takfiri network were also nabbed in March on suspicions of calling for attacks in Spain and trying to recruit for the ISIL.
Spanish authorities believe that about 100 people from the country have joined Takfiri terrorists in Iraq and Syria.
The ISIL militants control parts of Syria and Iraq, and have been carrying out horrific acts of violence such as public decapitations and crucifixions against all communities.
The US National Counterterrorism Center (NCTC) said in an estimate on February 10 that more than 20,000 individuals from around the world, including some Americans, have traveled to Syria to join the ISIL and other extremist groups.
Foreign militants from over 90 countries, including at least 3,400 people from Western states and more than 150 Americans, have traveled to Syria to join the terrorist groups there, the NCTC added.
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