It was once a monastic retreat, and dotted throughout the forest are secret grottoes, waterfalls, fountains, and tiny hermitages. Women were banned from this "garden of Eden" by papal decree to keep the monks free from temptation, and anyone who destroyed a tree was threatened with excommunication. On the exterior façade of a 17th century Rococo gate to the forest, the Coimbra Gate, are two marble plaques displaying the text of these two papal bulls.

One of the major battles of the Peninsular War took place here, when the Duke of Wellington defeated Napoleon's troops in 1810. Outside the forest wall, a small museum dedicated to the Peninsular War explains the Napoleonic invasion through engravings, maps, uniforms, and weapons. Just above it is an obelisk standing as a memorial to the battle.

In the center of it all is the neo-Manueline Buçaco Palace, one of Europe's most grandiose smaller palaces. It is now one of the country's top hotels and one of Europe's oldest. Commissioned by King Carlos in 1888, it began as a royal hunting lodge and was only used once by his son Manuel II. He stayed at the palace with French actress Gaby Deslys, with whom he had a brief romance before his exile in 1910. Soon after that, in the years between the two world wars, it became one of Europe's most fashionable addresses for socialites as a luxury hotel.