A 30-kilometre (20-mile) long line of fires was moving towards Athens, reports said, and one has already engulfed the mountain, also known as Mount Pentelikon, famed for the marble used in the Acropolis and other ancient buildings in Athens.
The nearby historic town of Marathon has also been ordered evacuated.
Brick homes on roads leading out of Marathon had huge black stains up the sides of their walls left by the flames. Their roofs had been turned to cinders.
"It's a catastrophe," said Marathon social worker Maria Kanavaki. "It's all burnt. There is a fear what will happen. This summer was the hottest. And the water -- will we have enough water?" the 55-year-old told AFP.
- 'Trauma in the area' -
Kanavaki recalled a disaster six years ago in the nearby seaside community of Mati, where fires killed more than 100 people -- some burned to death in their cars while trying to flee.
Kanavaki said people were still in "trauma". "They are still crying. So it's not easy to face all this again... I'm worried about the people".
Two volunteers brought seven cats into Marathon's cultural centre. Ivan Mahmood, a delivery driver, said he had been told by authorities to help rescue animals and found that most owners were elderly and had no car to escape.
"They are old men and women in the villages," said Mahmood. "They're in shock but they don't want to leave. They think if they stay, the fire won't come," the 27-year-old resident of nearby Nea Makri told AFP.
At Dione, the fire burned cars and crept up the walls of apartment blocks. Some residents said they fled in their cars just as the flames sped up to their homes.
People in Penteli, an Athens suburb at the foot of the 1,109-metre (3,605-foot) Mount Pentelicus, could only watch helplessly as fierce summer winds pushed flames toward their homes and up the slopes.
Thick smoke from burning trees filled a Penteli quare where local resident Mariana Papathanasi said they could only pray that their houses would be spared.
- Hospitals evacuated -
"Some houses were burned after midnight and we are trying to protect our local restaurant," the 49-year-old supermarket employee told AFP.
A children's hospital and a military clinic in Penteli were evacuated at dawn as Greek authorities ordered thousands of people in Marathon and surrounding villages to flee.
"The firefighters are doing very well," said Papathanasi. "They are close to us, the local people, the whole time." At least five fire trucks and several firefighters, some in heavy-duty masks, worked nearby.
Farther up the mountain, on the road to Nea Makri, tall flames devoured trees and shrubs, turning the ground black as grass and trees swayed wildly in the wind.
Christoforos, 53, a volunteer firefighter from Penteli, said the fires were moving fast and Nea Makri could become a major problem as two large fire fronts could meet there.
Greek authorities have thrown hundreds of firefighters with trucks and water carrying aircraft into what has become an annual battle as global temperatures soar.
After the warmest winter on record, Greece also experienced its hottest June and July since reliable data collection began in 1960, and the summer season has already seen repeat blazes.
Temperatures around Athens were forecast to peak at 39 degrees Celsius (102 degrees Fahrenheit) on Monday, with wind gusts of up to 50 kilometres (31 miles) per hour.
Scientists say that human-induced fossil fuel emissions are worsening the length, frequency and intensity of heatwaves around the world.
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