"The guerrilla war is history," said Chavez, speaking during his weekly television and radio program, "Hello President."
"At this moment in Latin America, an armed guerrilla movement is out of place."
Such declarations were unexpected from Chavez, a self-described socialist who earlier this year called on world governments to remove the FARC from terrorist lists and suggested the guerrillas should be recognized as a legitimate insurgent force.
Addressing new FARC leader Alfonso Cano, Chavez said, "I think the time has come to free all of the hostages you have. It would be a great, humanitarian gesture. In exchange for nothing."
In the past, the guerrillas have said they would be willing to release hostages in exchange for imprisoned guerrillas in Colombia and the United States.
Carlos Lozano, who in the past has acted as a mediator between the rebels and the government, told Caracol radio Sunday that he had re-established contact with the FARC in the hopes of facilitating hostage releases.
Lozano, the editor of a communist newspaper, said that while he had not spoken directly with Cano, "everything is going the right way".
But a FARC statement posted Sunday on a sympathetic Web site suggested the group was far from considering laying down its arms.
Written by rebel leader Luciano Marin Arango, alias Ivan Marquez, and dated June 5, the statement demanded that new elections be called to oust Colombia's government and Congress.
The FARC's "strategic objective is the taking of power for the people," the statement said.
Marquez also claimed that Colombian President Alvaro Uribe is overseeing plans to kill Chavez and leftist Ecuadorean President Rafael Correa.
The Colombian government did not respond immediately.
Recent efforts to free high-profile hostage Ingrid Betancourt and others have failed. The situation worsened when Colombia waged a cross-border raid on a rebel camp in Ecuador in March that killed a FARC leader.
The raid prompted both Chavez and Correa to send troops briefly to their respective borders with Colombia. Ecuador went a step further and cut off diplomatic relations, which still have not been restored fully.
But on Sunday, Chavez apparently changed his tune.
"You in the FARC should know something: You have become an excuse for the empire to threaten all of us," he said, using his frequently employed term for the United States. "The day that peace arrives in Colombia, the empire will have no excuses."
The Venezuelan leader's comments could help improve diplomatic relations with Colombia, which have been strained for months due to Colombia's allegations that Chavez could be aiding the FARC.
Chavez repeatedly has denied secretly supporting the FARC, saying his government's contacts with the guerrillas have been aimed only at securing the release of rebel-held hostages.
Meanwhile, Colombia's chief prosecutor said a Venezuelan National Guard officer and a second Venezuelan were among four people arrested while carrying tens of thousands of Kalashnikov rounds that Colombian authorities believe were destined for the FARC. The Kalashnikov is the FARC's standard-issue weapon.
Two of the men had Venezuelan identity papers and one claimed to be a sergeant in the national guard, prosecutor Mario Iguaran said in a statement Friday. The four were captured in eastern Colombia, close to the porous border with Venezuela.
Colombia's foreign minister has asked Venezuelan authorities to help investigate.
Inside Colombia, a huge arms black market supplies leftist guerrillas, right-wing death squads and the drug cartels.
In a statement issued Sunday, Venezuela's foreign ministry announced that authorities were cooperating with Colombia to help determine the identities of the two detainees.