• 3D printing enables fabrication of MSC electrodes with stable macrostructure and GA-crosslinked micropore structure.
• Surface modification with MoS2 nanosheets significantly enhances electrochemical performance.
• Achieved ultra-high areal capacitance of 3.99 F cm−2 and energy density of 1997 mWh cm−2.
• The method offers a simple, efficient route for high-performance MSC electrodes suitable for portable electronics.
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