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One-dimensional Al-doped CdS nanobelts were synthesized for the first time via chemical vapor deposition. The vertically synthesized Cd1-xAlxS nanobelts (x = 0–3.09) exhibited high crystallinity. We have reported here an investigation of optical and electrical properties of prepared nanobelts for potential applications in nano-optoelectronics. The successful incorporation of Al into individual CdS nanobelts was confirmed by powder X-ray diffraction analysis, energy-dispersive X-ray spectroscopy, and Raman spectroscopy. Photoluminescence spectra showed multiple peaks; one emission band appeared at 728 nm (red emission), and a new broad emission band consisting of three peaks centered at 930–961 nm (NIR-1), 954–992 nm (NIR-2), and 1042 nm (NIR-3) appeared in the near-infrared (NIR). All the NIR peaks correspond to the d–d transition of Al ions. Doping with 3.09% Al increased the conductivity of the samples from 1.097 × 10−6 to 2.59 × 10−5 A, indicating suitability for optoelectronic applications, including nanoscale light sources and buffer layer materials in solar panels.