A ministry statement said three Spaniards were arrested in Spain's North African enclave of Ceuta while a Moroccan was arrested in the nearby Moroccan city of Nador.
The ministry said the four formed a group that looked to recruit fighters to join IS in Iraq and Syria, as well as militants willing to carry out attacks in Spain and Morocco.
Spanish police arrested some 100 suspected Islamic extremists last year and more than 600 since the 2004 train bombings in Madrid that killed 191 people and injured nearly 2,000.
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