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Summary: All‐solid‐state flexible supercapacitors (FSCs) are promising energy‐storage devices in wearable smart electronics. Carbon cloth (CC) has emerged as an ideal candidate as it can fulfill all the required properties for conductive, corrosion‐resistant, and lightweight FSC substrates. However, commercial CC is difficult to adhere to without crosslinkers and binders owing to the hydrophobic surface. Herein, oxygen plasma and chemistry methods are selected for hydrophilic modification of commercial CC. Then, Ti3C2Tx flakes are coated on the surface of modified CC as active materials. These modified morphologies were characterized by scanning electron microscope and mechanical properties were investigated by a fabric tensile tester. The electrochemical properties of the MXene‐based electrodes by two modification methods were compared. Chemistry modification CC/Ti3C2Tx electrode exhibits an areal capacitance of 513 mF cm−2, which is 88% higher than that of oxygen plasma‐modified CC/MXene electrode, and capacitance retention remains above 92% after 10 000 cycles. This work proposes a feasible strategy, offering a platform for rational designs of flexible electronics based on textiles, as well as employing a large family of MXenes and their heterostructures. [ABSTRACT FROM AUTHOR]