Silicon anode undergoes dramatic volume expansion during charge and discharge, causing structural and interfacial instability that severely degrades battery cycling performance. Herein, we propose a three-dimensional (3D) flexible self-standing SiMP/SWCNT-COOH@PVA/PAA anode, in which carboxylation-modified single-walled carbon nanotubes (SWCNT-COOH) construct a highly conductive and flexible skeleton to provide rapid electron transport channels for micron silicon (SiMP), while polyacrylic acid-polyvinyl alcohol (PVA-PAA) cross-linking layer forms a high-strength polymer interface to strengthen the conductive skeleton and helps to maintain the structural integrity of SiMP. The resulting electrode exhibits ultra-high electrical conductance (12406 S m−1) and exceptional mechanical characteristic (tensile strength of 46.95 MPa). More importantly, it demonstrates extremely stable electrochemical properties, with an impressive maximum capacity of approximately 2868.5 mAh g−1 at 0.2C, while retaining an exceptional 96.49 % of capacity even after 100 cycles. A consistent capacity of 1000 mAh g−1 at 1C throughout 1000 cycles is also realized. Furthermore, a flexible full battery based on SiMP/SWCNT-COOH@PVA/PAA anode achieves a discharge capacity of 49.5 mAh g−1 following 100 cycles, and illuminates a LED strip normally under various bending conditions. These results are expected to open a new way towards enhanced performance silicon-based electrodes within flexible LIBs.