'We have seen links to drug trafficking and distribution, organised immigration crime, modern slavery and human trafficking, firearms, and the sale of illicit tobacco and vapes.
'We know cash-intensive businesses are used as fronts for money laundering, facilitating some of the highest harm and highest impact offending in the UK.
'The excellent results from the first iteration of Operation Machinize are testament to the tireless work of officers across the country, and demonstrate our resolve to clamp down on organised criminality abusing the high street.'
Security Minister Dan Jarvis said: 'High street crime undermines our security, our borders, and the confidence of our communities, and I am determined to take the decisive action necessary to bring those responsible to justice.
'This successful NCA-led operation highlights the scale and complexity of the criminality our towns and cities face and demonstrates our collective determination to make our streets safer, a key pillar of this government's Plan for Change.
'We will continue to support the NCA, and other law enforcement partners, as we make the UK an even more hostile environment for organised crime.'
The latest crackdown follows a spate of police raids on Turkish barber shops last month, which saw the seizure of more than £500,000 in illegal cash.
Seven people were arrested during the swoop on 33 premises by West Mercia Police, as part of the NCA's broader operation.
More than 750 barbers opened in the UK last year despite a widespread High Street downturn - raising suspicions that some are being used by gangs.
Detective Inspector Dan Fenn, of West Mercia Police's Economic Crime team, said previously: 'Organised crime groups are opportunistic and exploit legitimate businesses, such as barbershops, to hide their illegal cash flow.
'The high cash turnover of these businesses makes them ideal for disguising illicit activities.