"There were DEA agents who worked to conduct political espionage and to fund criminal groups so they could launch attacks on the lives of authorities, if not the president," Morales said.
The United States called Morales's allegations "false and absurd."
"We reject the accusation that DEA or any other part of the US government supported the opposition or conspired against the Bolivian government," State Department spokesman Karl Duckworth said in Washington.
"Should US cooperation be ended, more narcotics will be produced and shipped to Bolivia. The corrupting effects, violence, and tragedy which will result will mainly harm Bolivia as well as . . . neighboring Latin American countries, Europe, and West Africa," he added.
Bolivia-US relations have deteriorated in recent months as Morales's government limited DEA activities, including flights over Bolivia. The government later expelled the US ambassador over charges of spying and involvement in antigovernment protests in the eastern lowlands.
The United States in turn added Bolivia to its antinarcotics blacklist, causing a cut in trade preferences that Bolivian business leaders estimate could cost South America's poorest country as many as 20,000 jobs.
US antidrug officials and diplomats have denied any political involvement.
Morales's decision creates an unfortunate situation, DEA spokesman Garrison Courtney said in Washington, but added, "We will find other ways to make sure we keep abreast of the drug-trafficking situation through there."
Two DEA agents were pulled from the Chapare coca-growing region in September after Bolivian officials reported threats against them from coca growers in the area, a bastion of support for the president, who came to prominence as leader of a coca-growers union battling US eradication campaigns.
The United Nations estimates that Bolivia's coca crop increased 5 percent in 2007 - far below the 27 percent jump recorded in Colombia, a close US ally. Cocaine seizures by Bolivian police working with DEA agents had also increased dramatically during the Morales administration.