A novel stress-induced method to grow semimetallic Bi nanowires along with an analysis of their transport properties is presented. Single crystalline Bi nanowires were found to grow on as-sputtered films after thermal annealing at 260−270 °C. This was facilitated by relaxation of stress between the film and the thermally oxidized Si substrate that originated from a mismatch of the thermal expansion. The diameter-tunable Bi nanowires can be produced by controlling the mean grain size of the film, which is dependent upon the thickness of the film. Four-terminal devices based on individual Bi nanowires were found to exhibit very large transverse and longitudinal ordinary magnetoresistance, indicating high-quality, single crystalline Bi nanowires. Unusual transport properties, including a mobility value of 76900 cm2/(V s) and a mean free path of 1.35 μm in a 120 nm Bi nanowire, were observed at room temperature.