We present the effect of a coupling agent on the optoelectrical properties of few-walled carbon nanotube (FWCNT)/epoxy resin hybrid films fabricated on glass substrates. The FWCNT/epoxy resin mixture solution was successfully prepared by the direct mixing of a HNO3-treated FWCNT solution and epoxy resin. FWCNT/binder hybrid films containing different amounts of the coupling agent were then fabricated on UV-ozone-treated glass substrates. To determine the critical binder content (Xc), the effects of varying the binder content in the FWCNT/silane hybrid films on their optoelectrical properties were investigated. In this system, the Xc value was approximately 75 wt%. It was found that above Xc, the coupling agent effectively decreased the sheet resistance of the films. From microscopy images, it was observed that by adding the coupling agent, more uniform FWCNT/binder films were formed.