Police allege the men - aged 37 and 57 - went on a stealing spree between Saturday and Wednesday, accusing them of running the scam 18 times across NSW.
The fraud scheme allegedly involved one man approaching a victim and informing them there was an issue with the front of their car while encouraging them to open the bonnet to have a look acting as a decoy.
Their offsider would then go through the inside of the car and plunder wallets, purses, cash and cards, police said.
Assistant Commissioner Stacey Maloney said the pair had stolen about $50,000 over the five days and was a pattern detected overseas.
"It was really quite callous and certainly cowardly," she told reporters on Thursday.
"They identified their victims quite quickly, notably women, and these men were in their 40s so they were not someone that they appeared to be fearful of putting their trust in, almost operating as good Samaritans."
Most of the victims were over 60, with the eldest in their mid 80s.
The duo were arrested in Glenthorne, near Taree on the NSW mid-north coast, on Wednesday after travelling from Victoria.
They had been in the country on tourists visas since December 28.
Police said a search of the pair and their vehicle found $6000 in cash, passports, mobile phones, a laptop and a number of money transfer receipts.
Ms Maloney said police were still on the hunt for two other alleged accomplices, also with similar descriptions of being caucasian and in their mid 40s.
She noted the offenders appear to be part of a "broader organisational syndicate" that transfers money overseas.
The assistant commissioner said the crimes were distressing in their targeting of victims and showed an unusual pattern of defrauding used outside of Australia.
"It makes my blood boil," she said.
"Most people who are good, honest, hard-working citizens and they're just going about their business, shopping like we do every day, and scammed in the way that they have is quite disgraceful to be perfectly honest."
The arrested pair are accused of duping victims in car parks across 15 suburbs in Sydney along with Goulburn, Newcastle and Wagga Wagga.
They have been hit with 72 charges each relating to theft, fraud and entering a vehicle without consent. They are facing Bail Court later on Thursday.
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