"I assure my prayers for this beloved nation and express my closeness to the families who have lost their children in the streets," he said two days after four more protesters died, bringing the death toll to 89.
"I call for an end to violence and a peaceful and democratic solution to the crisis," the Argentine said at the end of the Angelus prayer in Saint Peter's Square.
No official details were provided as to what led to the latest deaths late Friday, although at least one opposition member of Venezuela's legislature said the victims, who ranged in age from 20 to 49, died by gunfire.
Saturday marks three months of opposition protests demanding the ouster of Venezuela's President Nicolas Maduro whose term in office runs until January 2019.
Maduro is blamed for a desperate economic crisis -- marked by shortages of food, medicine and other basics -- that has sparked hunger and deadly violence.
The international community has called for mediation to solve the Venezuela crisis after Vatican-backed talks last year broke down.
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