Their five-year-old daughter, who was injured in the incident, is said to be in a stable condition in hospital.
Police have launched an investigation into the killing, which happened on the highway leading from Valencia to Puerto Cabello.
Monica Spear, 29, became Miss Venezuela in 2004, and also acted in soap operas.
Local media reported that Monica Spear and her husband had stopped by the roadside because their car had broken down.
The gunmen opened fire in what police said might have been a robbery gone wrong.
Venezuela has one of the highest murder rates in the world, and armed robberies and kidnappings are not unusual.
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