Silicon has been investigated intensively as a promising anode material for rechargeable lithium-ion batteries. The choice of a binder is very important to solve the problem of the large capacity fade observed along cycling. The effect of modified elastomeric binders on the electrochemical performance of crystalline nano-silicon powders was studied. Compared with the conventional binder (polyvinylidene fluoride (PVDF)), Si electrodes using the elastomeric styrene butadiene rubber (SBR) and sodium carboxymethyl cellulose (SCMC) combined binder show an improved cycling performance. The reversible capacity of the Si electrode with the SCMC/SBR binder is as high as 2221 mA·h/g for 30 cycles in a voltage window between 0.005 and 2 V. The structure changes from SEM images of the silicon electrodes with different binders were used to explore the property improvement.