Four aircraft and 30 firefighters aided in attempts to control the blaze and additional forces were placed on alert while authorities blocked off Highway 1, the main road between Tel Aviv and Jerusalem.
Authorities said that there was no immediate threat to Hadassah Ein Kerem Medical Center.
The Ministry of Environmental Protection warned of dangerous levels of air pollution as the fireburned several buildings built with asbestos.
Nearby residents were asked to stay in their homes with windows closed and air conditioners off.
Firefighters were also dispatched near the Alon Moreh settlement in the West Bank where a fire had started.
Israel's largest fire since the devastating Carmel blaze in 2010 was extinguished near Beit Shemesh just over a week ago, after more than 150 firefighters and volunteers spent the day protecting homes in the villages of Tarum, Kfar Uriya and Ta'oz.