During a state of the nation address, he said that Eta's return to killing means "there is no margin to try" reviving a dialogue that he sought to establish after the "permanent" ceasefire in March 2006.
Eta violated the truce on December 30 with a bomb that killed two Ecuadorean men at Madrid airport.
The killings were the first credited to the group since May 2003 and took the death toll across four decades of Eta violence to 819, official government figures showed.
On June 5, Eta said it was resuming its armed campaign "on all fronts" in frustration at the lack of progress towards talks with the government, which it accused of failing to make any concessions.
In a related development, French anti-terrorist police arrested three suspected members of Eta on Monday as they prepared to cross into Spain in a van packed with explosives, police said.
The three were stopped at the French town of Saint Jean Pied de Port with more than 160kg of chemical explosives, two gas bottles, two detonators and an assault rifle.
The three men were arrested some 15km from the Spanish border.
One of the men handed over the van to the other two when police moved in. Their identities and destination in Spain were not immediately known.