Nanowires are important potential candidates for the realization of the next generation of sensors. They offer many advantages such as high surface-to-volume ratios, Debye lengths comparable to the target molecule, minimum power consumption, and they can be relatively easily incorporated into microelectronic devices. Accordingly, there has been an intensified search for novel nanowire materials and corresponding platforms for realizing single-molecule detection with superior sensing performance. In this work, progress made towards the use of nanowires for achieving better sensing performance is critically reviewed. In particular, various nanowires types (metallic, semiconducting, and insulating) and their employment either as a sensor material or as a template material are discussed. Major obstacles and future steps towards the ultimate nanosensors based on nanowires are addressed.