Flexible silicon/single-walled carbon nanotube (Si/SWCNT) composite paper was prepared using the pulsed laser deposition (PLD) method to deposit Si onto SWCNT paper. In the composite, Si mainly shows nanoworm-like morphology. Increasing deposition time results in an increased amount of Si microspheres. Electrochemical measurements show that the capacity of the composite paper is improved by the presence of Si. The Si/SWCNT composite with only 2.2% Si shows a capacity of 163 mA h g−1 at a current density of 25 mA g−1 up to 50 cycles, which is more than 60% improvement of the capacity of pristine CNT paper. The Si contribution in the 2.2%-Si/SWCNT sample is calculated to be higher than 3000 mA h g−1.