The arrests were made in and around Madrid in an operation co-ordinated with the FBI.
Police said millions of euros were taken from the victims, most of them in the United States and European Union.
Those targeted were wrongly told they had won a lottery and asked to send a payment before prize money could sent.
Thousands of letters and e-mails, most in ungrammatical English, were sent out to prospective victims every day, police said.
The faked documents asked them to make an initial payment of 900 euros ($1,400, £720) in taxes or administrative costs.
The scam is estimated to have netted around 20 million euros, but the actual sum could be many times that, say police.
Do people still fall for these Nigerian scams?
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