Separation of Li isotopes by laser deflection of atomic beams has been carried out. An atomic beam apparatus with a collimating ratio of 450/1 generates a Li atomic beam of 109 atoms/cm3 at the oven temperature of 600C. The CW tunable dye laser crossing the atomic beam at a right angle has a linewidth of 6 MHz and its intensity at the 1 cm interaction area is about 70 mW/cm2. When the laser frequency is tuned to coincide with 7Li 22P3/2F=3-22S1/2 F = 2 transition, TLi atoms are deflected from the beam. The deflected atoms are very pure 7Li and almost does not contain 6Li. When the laser frequency coincides with any other transition of 22P -22/S of both 6Li and 7Li, no apparent deflection is observed because of the optical pumping of the hyperfine levels of the 22/S1/2 ground state.