Troitino, 55, has been convicted of 22 murders, including a 1986 bombing in Madrid which killed 12 police officers, and had been on the run for over a year.
Lerin, 38, from Pamplona, is considered one of ETA’s most dangerous terrorists and has been on the run since April 2007, the ministry said.
The pair were said to be sharing a residence, living clandestinely in the capital and using false documents.
Both men are wanted by the National Court in Madrid, which specialises in terrorist cases.
Troitino, from the Palencia province of northern Spain, was one of ETA’s most prolific killers in the 1980s.
In July 1986 he detonated a car bomb by remote control in the Plaza de la Republica Dominicana in the Spanish capital. The blast destroyed a Civil Guard van, killing 12 officers and wounding 51 people.
He was arrested in 1987 and jailed for 2,232 years at the National Court in 1989.
There was public outrage when Troitino was released from prison in April last year after serving 24 years. Days later the National Court revoked his release and ordered him back to jail, but he went on the run before security services could locate him.
Spain’s Interior Ministry said the two men were arrested in a joint operation between the Metropolitan police and Spain’s National Police.
They said in a statement: “These two fugitives from the terrorist organisation ETA were on the security services’ most wanted list and are also wanted by the National Court.
”Troitino was responsible for more than 20 murders in a number of terrorist attacks.
”He is the subject of a European Arrest Warrant issued by the National Court, for belonging to a terrorist organisation.
”In 1985 he joined ETA’s terrorist cell in Madrid. This cell’s actions were particularly bloody, and they were responsible for the brutal attack against a Civil Guard bus which killed 12 Civil Guard officers and wounded 51 others.
”Lerin is the subject of an European Arrest Warrant issued by the National Court, for belonging to a terrorist organisation and possession of explosives.
”These arrests have dealt a powerful blow to ETA, as Antonio Troitino was a key figure in the terrorist organisation and had direct links with the current leadership of the terrorist group.
”The operation is ongoing.”
ETA has killed more than 800 people since it launched its campaign for an independent Basque state in the late 1960s.
In January last year the group announced a “permanent ceasefire” following more than 40 years of bloodshed.
The terrorist group is being urged to hand over its weapons and make a public apology to victims.
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