The rapid development of microelectronics has equally rapidly increased the demand for miniaturized energy storage devices. On‐chip microsupercapacitors (MSCs), as promising power candidates, possess great potential to complement or replace electrolytic capacitors and microbatteries in various applications. However, the areal capacities and energy densities of the planar MSCs are commonly limited by the low voltage window, the thin layer of the electrode materials and complex fabrication processes. Here, a new‐type three‐dimensional (3D) tubular asymmetric MSC with small footprint area, high potential window, ultrahigh areal energy density, and long‐term cycling stability is fabricated with shapeable materials and photolithographic technologies, which are compatible with modern microelectronic fabrication procedures widely used in industry. Benefiting from the novel architecture, the 3D asymmetric MSC displays an ultrahigh areal capacitance of 88.6 mF cm−2 and areal energy density of 28.69 mW h cm−2, superior to most reported interdigitated MSCs. Furthermore, the 3D tubular MSCs demonstrate remarkable cycling stability and the capacitance retention is up to 91.8% over 12 000 cycles. It is believed that the efficient fabrication methodology can be used to construct various integratable microscale tubular energy storage devices with small footprint area and high performance for miniaturized electronics.

High performance, flexibility, safety, and robust integration for micro-supercapacitors (MSCs) are of immense interest for the urgent demand for miniaturized, smart energy-storage devices. However, repetitive photolithography processes in the fabrication of on-chip electronic components including various photoresists, masks, and toxic etchants are often not well-suited for industrial production. Here, a cost-effective stamping strategy is developed for scalable and rapid preparation of graphene-based planar MSCs. Combining stamps with desired shapes and highly conductive graphene inks, flexible MSCs with controlled structures are prepared on arbitrary substrates without any metal current collectors, additives, and polymer binders. The interdigitated MSC exhibits high areal capacitance up to 21.7 mF cm −2 at a current of 0.5 mA and a high power density of 6 mW cm −2 at an energy density of 5 µWh cm −2. Moreover, the MSCs show outstanding cycling performance and remarkable flexibility over 10 000 charge-discharge cycles and 300 bending cycles. In addition, the capacitance and output voltage of the MSCs are easily adjustable through interconnection with well-defined arrangements. The efficient, rapid manufacturing of the graphene-based interdigital MSCs with outstanding flexibility, shape diversity, and high areal capacitance shows great potential in wearable and portable electronics.

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MoS2 has drawn great attention as a promising alternative to Pt-based catalysts for the hydrogen evolution reaction (HER). However, it suffers from sluggish kinetics to drive the HER process because of inert basal planes. Here, an on-chip MoS2 monolayer (MoS2 ML) HER reactor was designed and fabricated to reveal direct thermal enhancement of MoS2 ML for the HER. The thermal effects generated efficient electron transfer in the atomic MoS2 ML and at the interface between the electrolyte and the catalyst, leading to enhanced HER activity. The MoS2 ML measured at a higher temperature (60 °C) possesses a significantly enhanced HER activity with a lower overpotential (90 mV at current densities of 10 mA cm–2), lower Tafel slope (94 mV dec–1), and higher turnover frequency (73 s–1 at an overpotential of 125 mV) compared to the results obtained at room temperature. More importantly, the findings are attractive toward understanding the thermal effect on 2D monolayers as well as the development of next-generation electrocatalysts.