SCs and MSCs has been hindered by several issues. In particular, the synthesis, postreaction treatment, and instability of GO present processing challenges for widespread application. [ 14,22 ] In addition, the complex fabrication required for GO-based electrodes limits the cost potential and versatility of devices, particularly for MSCs with interdigitated structures. [ 4,23 ] Chemical vapor deposition has also been used to prepare graphene directly, but has limited scalability and often requires harsh synthetic conditions. [24][25][26][27][28][29] Laser scribing was recently developed to prepare porous graphene networks from polyimide. [ 30,31 ] This technology simplifi es the fabrication processes of MSCs compared to the photolithography approach, but still suffers from several limitations, such as limited compatibility with other substrates beyond polyimide and low energy storage ability. [ 4 ] Inkjet printing offers a desirable suite of advantages, including additive, non-contact, digital fabrication with high spatial resolution. Moreover, inkjet printing is an industrially mature technology, facilitating rapid transfer of technology from prototyping to manufacturing. The process and substrate compatibility achieved by this method, along with its commercial relevance, make the fabrication of microsupercapacitors by inkjet printing highly advantageous. However, challenges remain in the development of suitable graphene-based inks combining process compatibility and desirable electrical performance. Consequently, the development of a facile and scalable method for the fabrication of graphene electrodes for high-performance SCs and MSCs remains an outstanding challenge.Recent reports have demonstrated liquid-phase exfoliation of graphite for the production of stable graphene dispersions using the polymer ethyl cellulose in common, low-cost solvents such as ethanol and terpineol. [32][33][34][35] The graphene/ethyl cellulose (G/EC) system is suitable for applications in scalable fl exible electronics, with demonstrated processing ease and compatibility with a range of desirable substrates, as well as excellent electrical conductivity and mechanical fl exibility. Moreover, this system can be tailored for a range of additive manufacturing technologies including inkjet, gravure, and screen printing. [ 32,36 ] Herein, we extend this promising processing platform to electrochemical energy storage applications, realizing high-performance solid-state SCs. The suitability of the G/EC material for all-solid-state SC applications is fi rst evaluated using blade-coated and spin-coated thin-fi lm electrodes in sandwich-structured devices. In this confi guration, the high-conductivity, binder-free electrode mitigates the need for a separate current collector, simplifying the device fabrication process and eliminating potentially weak interfaces to enable Advances in thin-fi lm energy storage technologies are required to power the emerging fi eld of printed and portable electronics, with applications spanning biomedical and en...