The five are believed to belong to a gang called the "Zorros Viejos", or "Old Foxes", which is accused of causing over USD 209,000 worth of damage to train carriages across the country.
The well-organised group would stop a train dead by pulling its security levers "which caused the convoy to break violently, with the consequent risk of injuries to passengers," police said in a statement yesterday.
"Once the train was stopped they would open and block the doors and descend to the tracks, where they would paint the carriages," the statement added.
The five suspects have been charged with four offences of public disorder and 54 counts of damage to property.
They are thought to have acted in Madrid, the central city of Cuenca, the Mediterranean port of Valencia and Cadiz in the southwest.
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