Eight people were detained during the operation which was carried out by police intelligence services and the Spanish Civil Guard.
"The dismantled Spanish-Moroccan network was, according to police investigations, responsible for sending jihadists to groups affiliated with al-Qaeda in Syria," the Spanish interior ministry said Friday in a news release.
Dozens of people, including minors, had been sent from the enclave and other parts of Morocco by the network, the ministry said.
Militants, almost from all around the Middle East, Africa and Europe, go to fight alongside terrorist groups in Syria, forming an unprecedented insurgency which has already taken tens of thousands of lives.
The Syrian government has long warned the United States and its western and regional allies against consequences of the war, already marked with brutality and hatred killings, to put the whole region in jeopardy.
A recently published study reveals that between 2,000 and 5,500 foreign nationals are active in Syria.
The UK, Ireland and France are among the EU countries estimated to have the highest numbers of fighters in Syria.
French Interior Minister Manuel Valls admitted Friday that of that number at least 120 militants are from France.