Single-crystal bismuth thin films 1 to 20 micrometers thick were fabricated by electrodeposition and suitable annealing. Magnetoresistance up to 250 percent at 300 kelvin and 380,000 percent at 5 kelvin as well as clean Shubnikov-de Haas oscillations were observed, indicative of the high quality of these films. A hybrid structure was also made that showed a large magnetoresistive effect of 30 percent at 200 oersted and a field sensitivity of 0.2 percent magnetoresistance per oersted at room temperature.