Operation Podium, the Metropolitan police unit dealing with organised crime connected to the Olympics, said that the fraudsters had targeted victims via an online dating website.
In a version of an online scam that officers said was becoming increasingly prevalent, the victims were persuaded to pay the "initial costs" of fulfilling a contract to supply coach transportation for police officers at the Olympics.
One victim, a 69-year-old woman from the US, was persuaded to part with £140,000 by the fraudsters. Scotland Yard worked with US law enforcement agencies on the operation.
"We are concerned that fraudsters have been using the name of the Met to foster increased levels of trust in their victims. Would-be fraudsters should be warned that we will investigate attempts to defraud the public in this way tirelessly," said Det Supt Nick Downing.
"At the same time we would urge the public across the world not to fall victim to these or any similar schemes. Suspect anyone you don't know personally who is asking for money in this way and who uses the name of a well known organisation, such as ours, in an attempt to add credence to their claims."
Tuesday's arrest follows previous arrests at the end of December of a 49-year-old man and a 39-year-old woman in connection with the case, who have been bailed until late March pending further inquiries.
The home secretary, Theresa May, said last week that Operation Podium had already made almost 100 arrests connected to organised crime linked to the Olympics. Offences are believed to include fraud and ticket touting.
Officers are concerned that criminals will use the London Games as a front for online fraud. As with other high-profile sports and entertainment events where tickets are at a premium, there is concern that potential purchasers will be tempted to buy tickets that may not even exist from unofficial websites.
Police and 2012 organisers have tried to emphasise that potential purchasers should only attempt to buy tickets from the official website, or through authorised European resellers.
"The police are working against cybercriminals, with a dedicated police operation against those who would seek to illegally profit from the Games," said Mrs May.
"That operation has already made nearly 100 arrests of organised criminals and work continues behind the scenes."
Guardian Unlimited
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