This thesis examines the architectural history of University College London (UCL) from its foundation to 1939. UCL traces its beginnings to 1825, when a group of radical thinkers set about establishing a secular, non-residential metropolitan university. Its first architectural expression was the grand neoclassical building constructed in 1827–9 to designs by William Wilkins. Only the central block, portico and dome of Wilkins’s scheme were completed, yet successive wing extensions gradually formed a neoclassical quadrangle in Gower Street. A hospital was built in 1833–4, securing space for clinical teaching. UCL was initially denied a charter and precluded from awarding degrees, a complication that was resolved by the creation of the University of London as a separate examining body in 1836. Over the next century, UCL and its hospital expanded in a gradual and piecemeal manner in line with advances in education, technology and healthcare. UCL’s estate became increasingly complex, with a mixture of purpose-built blocks and the adaptation of buildings in the vicinity. A wealth of archival records, along with documentary sources and field investigation, has been used to examine the historic core of UCL’s estate in Bloomsbury. Institutional identity and aspirations are analysed in concert with practical influences on building projects, such as finances and functionality. The matter of identity also arises in the attribution of buildings to specific architects, which points to a tradition of enlisting professors such as Thomas Leverton Donaldson, Thomas Hayter Lewis, Thomas Roger Smith, Frederick Moore Simpson and Albert Richardson. In practice, their work was informed by multiple voices such as committee members, academic staff, external consultants and benefactors. This research addresses significant gaps in knowledge of the buildings, planning and development of UCL, while considering issues of identity, attribution and methodology pertinent to the study of architectural history.