Binder-free electrodes employed in supercapacitor devices can exhibit excellent electrochemical performances due to the improvement of electronic conductivity and the utilization rate of electrode materials. However, a simple, efficient and tunable strategy for preparation of binder-free MXene-based electrodes, especially for developing a general method for fabricating the MXene-based wearable flexible supercapacitors, still remains a challenge to meet the requirements of practical applications. In this study, we fabricated binder-free MXene-based films with adjustable mass loading and reduced agglomeration on the nickel foam and wearable flexible fabric substrates by the modified electrophoretic deposition method using organic colloid containing few-layers Ti3C2Tx nanoflakes. Their electrochemical performances are studied by cyclic voltammetry, galvanostatic charge-discharge and electrochemical impedance spectroscopy, respectively. The binder-free electrodes can deliver high capacitance (∼140 F g−1 in alkaline electrolyte), stable cycling performance with no capacitance loss after 10,000 cycles and good rate performance, which can be attributed to the reduced agglomeration of Ti3C2Tx films with a layer-by-layer self-assembled stackable structure, optimized pore-size distribution (∼4 nm) and excellent electronic conductivity, enhancing the accessibility to electrolyte ions and enabling full utilization of the MXene nanoflake surfaces.