A Hom-structure on a Lie algebra (g,[,]) is a linear map σ W g σ g which satisfies the Hom-Jacobi identity: [σ(x), [y,z]] + [σ(y), [z,x]] + [σ(z),[x,y]] = 0 for all x; y; z ∈ g. A Hom-structure is referred to as multiplicative if it is also a Lie algebra homomorphism. This paper aims to determine explicitly all the Homstructures on the finite-dimensional semi-simple Lie algebras over an algebraically closed field of characteristic zero. As a Hom-structure on a Lie algebra is not necessarily a Lie algebra homomorphism, the method developed for multiplicative Hom-structures by Jin and Li in [J. Algebra 319 (2008): 1398–1408] does not work again in our case. The critical technique used in this paper, which is completely different from that in [J. Algebra 319 (2008): 1398– 1408], is that we characterize the Hom-structures on a semi-simple Lie algebra g by introducing certain reduction methods and using the software GAP. The results not only improve the earlier ones in [J. Algebra 319 (2008): 1398– 1408], but also correct an error in the conclusion for the 3-dimensional simple Lie algebra sl2. In particular, we find an interesting fact that all the Hom-structures on sl2 constitute a 6-dimensional Jordan algebra in the usual way.