Dodgy barbers, vape stores and mini-marts will be shut down in a £30million crackdown led by 'Britain's FBI'.
A new High Street Organised Crime Unit, announced by Home Secretary Shabana Mahmood, will target money laundering, illegal working and tax evasion.
The scheme will aim to carry out thousands of raids, seize cash and close down criminal operators, with the National Crime Agency estimating crooked high street businesses are responsible for laundering £1billion a year.
It comes amid claims corner shops are taking payments for small boat traffickers.
Smugglers have been collecting money for illegal Channel crossings using a network of UK-registered businesses, a BBC investigation found.
Staff at a shop in Woolwich, south-east London, were secretly filmed telling an undercover researcher that nearly £3,000 in cash could be deposited with them and transferred to a smuggler in France.
The trafficker also provided undercover reporters, who were posing as migrants, with bank account details of two UK-registered companies – a wholesaler in Newcastle upon Tyne and a Cambridgeshire car wash - which he said could take electronic transfers for migrant crossings.
The Home Office's new unit will bring together the NCA, police, the taxman and trading standards.
Home Secretary Shabana Mahmood said the new £30million operation would crack down on criminal gangs which 'exploit our high streets to launder their dirty money' and 'undercut honest businesses'
Dodgy high street businesses have been taking payments for illegal Channel crossings from the Continent, a BBC investigation found
It will target a variety of businesses including America-style 'candy stores' – such as those in London's West End – which have been implicated in money laundering, selling counterfeit goods, overcharging tourists and failing to pay business rates.
The Home Secretary said: 'Criminal gangs have exploited our high streets to launder their dirty money and undercut honest businesses.
'We are hitting back with a nationwide crackdown to shut these fronts down, seize dirty cash and drive organised crime off our high streets and put bosses behind bars.'
NCA deputy director of illicit finance, Sal Melki, said it would aim to 'get this criminal element out of our high streets'.
The new scheme will aim to expand the work of an 18-month NCA operation which has seen 950 arrests and more than £10million of criminal assets seized.
Estimates by the agency say at least £12billion of criminal cash is generated in the UK each year, with £1billion laundered through high street businesses.
The Home Office said the three-year programme will see 75 new police officers recruited across the NCA, Greater Manchester Police, West Midlands Police and a joint Kent Police and Essex Police Unit, to 'build intelligence at a national level and increase the number of dedicated officers tackling organised crime on the ground'.
Funding includes £20million to the NCA and the National Police Chiefs' Council, £6million to trading standards departments, £1.5million to the Home Office's Immigration Enforcement agency and £1.35million to HM Revenue and Customs.
A further £900,000 will go on running the unit based in the Home Office, with the scheme overseen by security minister Dan Jarvis.
It could lead to recommendations for new legal powers to tackle organised crime on the high street.
Chief executive of the British Retail Consortium, Helen Dickinson, said: 'Stolen goods are commonly funnelled through illicit supply chains and resold through unscrupulous businesses, helping fund further criminality.
'This harms businesses, puts colleagues at risk, and pushes up prices for honest shoppers.
'Tackling it requires prioritisation from police and government, and co-ordination and intelligence sharing between retailers, law enforcement, and local partners.
'We look forward to working together to deliver real progress.'
Chris Philp, Shadow Home Secretary, said: ‘Labour have done more damage to our high streets than 75 officers can fix.
‘Under Labour, there are 1,300 fewer police officers, a huge spike in business rates, anti-business legislation, jobs tax, the list goes on.
‘Crime and antisocial behaviour are at unacceptably high levels, every day, too many people witness things that anger and alarm them.
‘The Conservatives have a plan to Take Back our Streets that would put 10,000 extra police officers on the streets, backed by £800 million, in order to triple stop and search, roll out live facial recognition to the worst crime hotspots, restoring the damage Labour have done in just under two years.’