• 3D printing enables fabrication of microsupercapacitor electrodes with stable macrostructure and GA-crosslinked micropore structure, achieving ultra-high areal capacitance of 3.99 F cm−2.
• Surface modification with MoS2 nanosheets significantly enhances electrochemical performance, yielding high energy density of 1,997 mWh cm−2 and power density of 194 μW cm−2.
• The interleaved grid structure and high mass loading of active material promote rapid ion and electron transport, addressing limitations of traditional 2D thin-film electrodes.
• This simple and efficient method offers a promising route for producing high-performance MSC electrodes suitable for portable electronic devices.