The crime-fighting agencies will share sensitive financial information on individuals and keep an eye on each other's operations through the exchange of personnel.
The deal expands an earlier arrangement agreed in 2002 between Europol and the US Department of Justice.
"We hope to work together more closely on areas like counterfeit money, financial crime and fraud, and exchange information about criminal suspects and networks," a Europol spokesman said.
Europol has already posted two liaison officers to Washington, while the US Secret Service has placed one person at Europol, the agency said.