The cloisters in the Main Quadrangle

The main campus is spread across two inner-city suburbs of Sydney: Camperdown and Darlington.
Originally housed in what is now Sydney Grammar School, in 1855 the government granted the university land in Grose Farm, three kilometres from the city, which is now the main Camperdown campus. The architect Edmund Blacket designed the original Neogothic sandstone Quadrangle and Great Tower buildings, which were completed in 1862. The rapid expansion of the university in the mid-20th century resulted in the acquisition of land in Darlington across City Road. The Camperdown/Darlington campus houses the university's administrative headquarters, and the Faculties of Arts, Science, Education and Social Work, Pharmacy, Veterinary Science, Economics and Business, Architecture, and Engineering. It is also the home base of the large Faculty of Medicine, which has numerous affiliated teaching hospitals across the state.

The main campus has been ranked among the top 10 of the world's most beautiful universities by the British Daily Telegraph.
The university is currently undertaking a large capital works program with the aim of revitalising the campus and providing more office, teaching and student space.
The program will see the amalgamation of the smaller science and technical libraries into a larger library, and the construction of a central administration and student services building along City Road. A new building for the School of Information Technologies opened in late 2006 and has been located on a site adjacent to the Seymour Centre. The busy Eastern Avenue thoroughfare has been transformed into a pedestrian plaza and a new footbridge has been built over City Road. The new home for the Sydney Law School, located alongside Fisher Library on the site of the old Edgeworth David and Stephen Roberts buildings, has been completed.