There is an urgent need for improved sorbents for the capture of carbon dioxide from the atmosphere, a process known as direct air capture. In particular, low-cost materials that can be regenerated at low temperatures would overcome the limitations of current technologies. In this work, we introduce an electrochemical method for preparing designer “charged-sorbent” materials and synthesise a hydroxide-functionalised activated carbon that can rapidly capture carbon dioxide from ambient air via (bi)carbonate formation. Unlike traditional bulk carbonates, material regeneration can be achieved at low temperatures (100 ºC), and the sorbent's conductive nature permits direct Joule heating regeneration. Given their highly tailorable pore environments and low cost, we anticipate that charged-sorbents will find numerous potential applications in chemical separations, catalysis, and beyond.