In this paper the author derives a geometric characterization of totally isotropic Willmore two-spheres in S6,which also yields to a description of such surfaces in terms of the loop group language.Moreover,applying the loop group method,he also obtains an algorithm to construct totally isotropic Willmore two-spheres in S6.This allows him to derive new examples of geometric interests.He first obtains a new,totally isotropic Willmore two-sphere which is not S-Willmore(i.e.,has no dual surface)in S6.This gives a negative answer to an open problem of Ejiri in 1988.In this way he also derives many new totally isotropic,branched Willmore two-spheres which are not S-Willmore in S6.