The thieves targeted luxury fountain pens as they traveled to shopping centers in Spain.
Three of the crew members were arrested by the Policia Nacional in Madrid.
Two more warrants are issued. One of the two is currently in Spain.
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They committed thefts in Alicante, A Coruña, and Oviedo with some Montblanc-branded pens worth as much as €9,800.
Two months ago, an attempted robbery in a shopping centre in Alicante sparked investigations.
11 pens worth over €8,000 were taken, but when fleeing, they left behind a backpack with 40 pens valued at over €28,000.
A high-value heist in A Coruña yielded 39 pens with a total €39,000 tag, and they are also accused of stealing eight cameras worth €8,602 from an Oviedo shop.
The Policia Nacional reported that the robberies had been coordinated by mobile phones, with gangs deployed in shopping malls performing distinct roles.
Some shop employees distracted while others forced display cases open.
After the robbery, other crew members took charge of diverting tactics.
The authorities said it was difficult to find the homes of gang members because they moved around and forged documents.