The 14 prisoners accused President Nicolas Maduro's socialist government of breaking promises made during fragile Vatican-backed negotiations with the opposition.
"Due to the regime's failure to honor the accords that it accepted in the talks, such as the freeing of the political prisoners, the setting up of a humanitarian supply channel and elections... We have decided to start a hunger strike," they said in a statement today.
The dialogue aims to calm tensions as the center-right opposition demands a vote on removing Maduro.
Maduro says the crisis is a US-backed capitalist conspiracy.
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He has rejected talk of holding a vote before the next general elections, scheduled in late 2018.
The latest round of talks between the two sides is scheduled for tomorrow. But it is unclear whether the opposition will attend.
The opposition MUD coalition has been divided over whether to hold talks with Maduro.
Those of its leaders that are taking part have threatened to abandon the "dialogue" if the government does not release the prisoners among other demands.
"We call on our fellow political prisoners being held in other prisons to join in" with the hunger strike, they said.
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