In this report, we describe a method for modifying electrical and optoelectrical properties of CdS nanobelts using low-energy (lower than 10 keV) e-beam irradiation in a scanning electron microscope. The electrical conductivity of the nanobelts was dramatically improved via the irradiation of e-beams. The modified conductivity of the nanobelts depends on the energy of the e-beam; it exhibits a larger photocurrent and higher external quantum efficiency but slower time-response than that before the modification. A possible mechanism about the modification is the increase of electron accumulation (injected electrons) in the nanobelts due to e-beam irradiation. In addition, the optoelectrical modification could be caused by the trapped electrons in the nanobelts and the decrease of contact resistance between the nanobelts and metal electrodes induced by e-beam irradiation. The results of this work are significant for the in situ study of semiconductor nanostructures in the electron microscope. Besides, the method of electrical and optoelectrical modification presented here has potential application in electronics and optoelectronics.