The 27-year-old man was attempting to cross into Spain from the country's enclave of Melilla on the North African coast and the suitcase was inside the trunk of his brother's car, who has been arrested.
The migrants have been left with nowhere to go after being evicted from the Tangier neighborhood of Boukhalef during a police raid last week.
The arrests are directly related to an operation that broke up another network last December that was recruiting young women and sending them to join radical militants in Syria and Iraq.
Some 600 migrants who had learned of the impending raid stormed the fence around Melilla to try and cross into Europe.
Thousands of migrants make dangerous crossings each year to the Spanish enclaves of Ceuta and Melilla in North Africa, which are seen as gateways for immigration to Europe.
A Spanish judge jailed four suspects who were allegedly part of a jihadist network that has managed to send 12 people to fight with the Islamic State in Syria and Iraq.
Ceuta is a small Spanish-administered town in North Africa separated from mainland Spain by the intersection of the Atlantic Ocean and the Mediterranean Sea. Many Syrian refugees have gotten caught trying to sneak onto the mainland from Ceuta and...
Some 1,600 sub-Saharan migrants have jumped across a fence that separates Africa from Europe since the beginning of the year.
More than 200 sub-Saharan migrants managed to climb over a triple-layer border fence into Spain’s North African enclave of Melilla.