This overview and synthesis paper focuses on the evolution of urban biogeochemical cycles across time. We synthesize empirical data and review existing literature, including papers in this special issue, and we propose the concept of “urban evolution.” The built environment often changes quickly in response to human activities, thus contributing to an urban evolution that affects structure, function, and ecosystem services of human settlements over time. Depending upon management, these changes can result in rapid losses of ecosystem functions/services or progress towards restoration. We explore urban evolution through empirical examples such as: (1) land development and nitrogen inputs within a metropolitan region over half a century; (2) watershed drainage by different forms of stormwater management over decades; (3) human-accelerated weathering in urbanized watersheds over decades; and (4) global salinization of freshwater across urbanizing landscapes over a century. We also synthesize concepts relevant to studying urban evolution of infrastructure and ecosystems including: (1) urban watersheds have challenged our whole notion of the “watershed approach” due to complex hydrologic boundaries and flow paths over time; (2) the urban hydrologic cycle evolves due to changing infrastructure and human water use over time; (3) the importance of extending research beyond individual sites using an urban watershed approach over space and time; (4) salinization as a universal tracer of watershed urbanization over time; (5) human-accelerated weathering of concrete and construction materials contributing to an “urban karst” over time; (6) human alteration of the carbon cycle in urban watersheds over time; and (7) detecting distinct biogeochemical signatures across cities globally over time. Our synthesis and this special issue suggest that urban biogeochemical cycles have exerted a major influence on the elemental composition of the Earth’s surface from local to global scales. A new global research agenda is needed to track the evolution of urban biogeochemical cycles as land development proceeds and infrastructure/management changes so we can better evaluate potential losses in ecosystem services, set realistic watershed and river restoration goals, and formulate effective environmental policy for Earth’s growing urban population.