A major transition to electric vehicles (EVs) is underway globally, as countries target reductions in greenhouse gas emissions from the transport sector. As this rapid growth continues, significant challenges remain around how to sustainably manage the accompanying large volumes of waste from end-of-life lithium-ion batteries that contain valuable rare earth and critical materials. Here, we show that high-shear exfoliation in aqueous surfactants can upcycle spent graphite anodes recovered from an EV into few-layer graphene dispersions. For the same hydrodynamic conditions, we report a process yield that is 37.5% higher when using spent graphite anodes as the precursor material over high-purity graphite flakes. When the surfactant concentration is increased, the average atomic layer number reduces in a similar way to that of high-purity precursors. We find that the electrical conductance of few-layer graphene produced using the graphite flake precursor is superior and identify the limitations when using aqueous surfactant solutions as the exfoliation medium for spent graphite anode material. Using these nontoxic solution-processable nanomaterial dispersions, functional paper-based electronic circuit boards were fabricated, illustrating the potential for end-to-end, environmentally sustainable upcycling of spent EV anodes into new technologies.