Li0.067Na0.933　Tb(MoO4)2　magneto-optical　crystal　was　grown　by　the　Czochralski　method.　The　effective　segregation　coefficient　of　Li+　in　NaTb(MoO4)2　was　measured.　The　lattice　parameters　of　the　crystal　were　determined　by　XRD　data.　Verdet　constants　of　Li0.067Na0.933Tb(MoO4)2　crystal　at　the　wavelength　532　nm,　633　nm　and　1064　nm　were　investigated　by　the　extinction　method　at　room　temperature.　They　are　-293.6　rad·m-1·T-1,　-200.5　rad·m-1·T-1　and　-68.6　rad·m-1·T-1,　respectively,　and　are　larger　than　that　of　pure　NaTb(MoO4)2　at　corresponding　wavelengths.　The　results　showed　that　Li0.067Na0.933Tb(MoO4)2　has　a　larger　magneto-optical　figure　of　merit　at　1064　nm　wavelength.