One of the 28 players took part in the last US Open, although their identity has not been revealed.
On the action day, 11 house searches were carried out in Spain in which €167,000 in cash was seized, alongside a shotgun, over 50 electronic devices, credit cards, five luxury vehicles and documentation related to the case.
Europol said at least 97 matches from lower-tier "Futures" and "Challenger" tournaments were fixed.
Europol said the players were among 83 people detained by Spain's civil guard, known as Guardia Civil, among them a tennis player who participated in the U.S. Open past year.
An independent review panel, set up by the sport's four governing organisations, the ATP, WTA, ITF and Grand Slam Board, last month published a report into the threat of match-fixing in the sport.
The European Sport Security Association has frequented listed tennis as the sport with the most suspicious betting alerts in its reports.
"A group of Armenian individuals used a professional player who served as the link between them and the other members of the network", the statement said, adding that 42 bank accounts were also frozen.
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"An organised crime group involved in manipulating professional tennis competitions was dismantled in an operation led by the Spanish Civil Guard and coordinated by the National High Court of Spain", Europol said in a statement.
The Armenian gang bribed players into fixing matches, according to authorities.
It was a warning by the Tennis Integrity Unit in 2017 that prompted Spanish authorities to begin the investigation.
The Armenian gang used a professional tennis player as the link between them and other players.
Authorities said members of the Armenian ring attended the matches to ensure the players complied with what was previously agreed.
Match-fixing has been a prominent issue in tennis recently, with Belgian prosecutors detaining 13 people in connection with the issue in June.