The element "lithium" has strong absorption lines near 6707.84 A and 3232.61 A and possesses specific isotope shifts at the respective absorption lines. With the aid of a laser capable of controlling the oscillation spectral width accurately to 0.01 A, the isotopes of this element are separated from each other by irradiating lithium atomic beam with a laser beam tuned to the absorption line of either of the isotopes, .sup.6 Li and .sup.7 Li, for thereby selectively exciting the isotope, ionizing the excited isotope along by irradiation with a laser beam having one photon energy enough to pump it from the excited state to the ionized state and separating the ionized isotope from the un-ionized isotope by means of a mass-filter.