Light-emitting electrochemical cells (LECs) can be fabricated with cost-efficient printing and coating methods, but a current drawback is that the LEC emitter is commonly either a rare-metal complex or an expensive-to-synthesize conjugated polymer. Here, we address this issue through the pioneering employment of metal-free and facile-to-synthesize carbon nanodots (CNDs) as the emitter in functional LEC devices. Circular-shaped (average diameter = 4.4 nm) and hydrophilic CNDs, which exhibit narrow cyan photoluminescence (peak = 485 nm, full width at half maximum = 30 nm) with a high quantum yield of 77% in dilute ethanol solution, were synthesized with a catalyst-free, one-step solvothermal process using low-cost and benign phloroglucinol as the sole starting material. The propensity of the planar CNDs to form emission-quenching aggregates in the solid state was inhibited by the inclusion of a compatible 2,7-bis(diphenylphosphoryl)-9,9′-spirobifluorene host compound, and we demonstrate that such pristine host-guest CND-LECs turn on to a peak luminance of 118 cd·m−2 within 5 s during constant current-density driving at 77 mA·cm−2.