Measurements of electrical resistivity and Hall coefficient of single‐crystal bismuth films evaporated on hot mica substrates, in the thickness range 250–1700 Å, were made at room temperature and 90°K. Resistivity and Hall coefficient of these films showed an oscillatory dependence on film thickness on account of the quantum size effect. The experimental period of the oscillations agrees with the theory of quantum size effect at these thicknesses. Detailed electron transmission studies were made to investigate the reported disagreement between experimental curves and theoretical predictions at small thicknesses. The role of structure on the behavior of resistivity and Hall coefficient of thinner films is discussed.