Nano-Si/(multi-wall carbon nanotube) (Si/MWCNT) composite paper was prepared as flexible electrode for lithium ion batteries by a simple filtration method using sodium carboxymethyl cellulose (CMC) as a dispersing/binding agent, followed by a thermal sintering process. Scanning electron microscopy (SEM) showed that nanosized Si particles were dispersed homogeneously and intertwined by the MWCNT throughout the whole paper electrode. After thermal sintering, Si/MWCNT paper electrode exhibited a significantly improved flexibility with a high Si content of 35.6wt% as compared with before sintering, and retained a specific capacity of 942mAhg−1 after 30 cycles with a capacity fade of 0.46%/cycle.