One man was arrested in Altea, just ten minutes down the coast from Benidorm on Wednesday morning, while another was held in Ceuta and two more in Morocco in a joint anti-terrorist operation.
The four men, of Moroccan nationality, are all suspected of links to militant Islamist activity, the Spanish Interior Ministry said.
The raid was carried out on a halal butcher shop just 100 meters from the beach in Altea.Photo: F Govan
Police said they formed two cells and had sworn loyalty to terror group Isis and were ready to carry out terrorist attacks.
The two arrested in Spain had assumed different roles according to the ministry statement. "One focused on brainwashing and radicalising potential jihadists and the other acted as an Internet-based charismatic leader, considered a sheik or spiritual leader by his disciples."
It added: "The risk the detainees posed was due not only to their capacity in terms of radicalising recruits, but also to their willingness to head to conflict zones and become martyrs or even commit terrorist acts in their countries of origen or the countries where they were living."
The arrests followed two years of police investigations and stemmed from monitoring two people who had lived in Spain but had gone to join Islamic State in Syria and Iraq, the ministry said in a statement.
These two formed a recruiting cell and then established off-shoots in Spain and Morocco, each containing a further two members.
The two men arrested in Spain were charged with enlisting and indoctrinating recruits to fight in Syria and Iraq with the use of social media. They had direct contact with Islamic State through the Syrian unit, the ministry said.
Two other suspected jihadists were arrested earlier in the week in northern Spain.
It brings the number of suspected Islamic terrorists arrested in Spain to more than 120 since the start of 2015.