Yes, exactly! The other operators that complete the basis can be given by the three operators $S_iS_j + S_jS_i$, one operator $S_x^2 - S_y^2$, and one operator $-1/\sqrt{3}(S_x^2+S_y^2-2S_z^2)$, as mentioned in
here on pp.4 in the context of tomography.