exhibited a modest areal energy density (<10 µWh cm −2 ). [5a] Thus, it is still a big challenge to efficiently and cost effectively fabricate asymmetric MSCs with high areal energy densities.Very recently, extrusion-based 3D printing, as an emerging technology, has been successfully demonstrated to construct complex structures with a wide application in various areas, such as electronic, [7] biomedical, [8] and energy storage fields. [9] To develop suitable inks with high viscosities and shear-thinning rheological properties, it is essential to print ideal architectures without collapse. During the printing process, the functional inks were extruded through nozzle and directly printed on substrates layer by layer in the vertical dimension. [10] To date, although 3D printing has been explored to build electrochemical architectures for lithium-sulfur batteries, [11] lithium-ion microbatteries, [12] and symmetric MSCs, [13] it is still in the initial stage to 3D print desirable devices with high electrochemical performances for energy storage applications.Here, we demonstrate that an asymmetric MSC with ultrahigh areal energy density can be facilely and precisely realized by the 3D printing technology. In a typical procedure, the cathode and anode inks are composed of vanadium pentoxide (V 2 O 5 ) and graphene-vanadium nitride quantum dots (G-VNQDs) with highly concentrated graphene oxide (GO) dispersions, respectively. The 3D printed asymmetric MSC with interdigitated electrodes exhibits excellent structural integrity, a large areal mass loading of 3.1 mg cm −2 , and a wide electrochemical potential window of 1.6 V. Moreover, there are substantial open macropores in the 3D printed electrodes, which can serve as numerous channels for accelerating the mass transportation. These features enable the 3D printed asymmetric MSC to have an ultrahigh areal energy density of 73.9 µWh cm −2 and power density of 3.77 mW cm −2 as well as a long cycle life up to 8000 cycles. Figure 1 illustrates the 3D printing procedures of the asymmetric MSC with interdigitated electrodes. The cathode (V 2 O 5 ) and anode (G-VNQDs) active materials were first synthesized according to our previously reported protocols (for details, see Supporting Information). [14] V 2 O 5 is considered as one promising cathode material due to its high Faradic activity and natural abundance, and VN is used as one anode materials owing to its large pseudocapacitance as well as appropriate negative operating potential. [15] Subsequently, cathode or anode ink was A 3D printing approach is first developed to fabricate quasi-solid-state asymmetric micro-supercapacitors to simultaneously realize the efficient patterning and ultrahigh areal energy density. Typically, cathode, anode, and electrolyte inks with high viscosities and shear-thinning rheological behaviors are first prepared and 3D printed individually on the substrates. The 3D printed asymmetric micro-supercapacitor with interdigitated electrodes exhibits excellent structural integrity, a large areal ...