On-paper microsupercapacitors (MSCs) are a key energy storage component for disposable electronics that are anticipated to essentially address the increasing global concern of electronic waste. However, nearly none of the present on-paper MSCs combine eco-friendliness with high electrochemical performance (especially the rate capacity). In this work, highly reliable conductive inks based on the ternary composite of poly(3,4-ethylenedioxythiophene): poly(styrenesulfonate) (PEDOT:PSS), graphene quantum dots and graphene are developed for scalable inkjet printing of compact (footprint area ≈ 20 mm2) disposable MSCs on commercial paper substrates. Without any post treatment, the printed patterns attain a sheet resistance as low as 4 Ω ▫−1. The metal-free all-solid-state MSCs exhibit a maximum areal capacitance > 2 mF cm−2 at a high scan rate of 1000 mV s−1, long cycle life (>95% capacitance retention after 10 000 cycles), excellent flexibility, and long service time. Remarkably, the “totally metal-free” MSC arrays are fully inkjet printed on paper substrates and also exhibit high rate performance. The life cycle assessment indicates that these printed devices have much lower eco-toxicity and global warming potential than other on-paper MSCs.
