We study several questions on the existence of negative Sasakian structures on simply connected rational homology spheres and on Smale-Barden manifolds of the form $#_k(S^2times S^3)$. First, we prove that any simply connected rational homology sphere admitting positive Sasakian structures also admits a negative one. This result answers the question, posed by Boyer and Galicki in their book [BG], of determining which simply connected rational homology spheres admit both negative and positive Sasakian structures. Second, we prove that the connected sum $#_k(S^2times S^3)$ admits negative quasi-regular Sasakian structures for any $k$. This yields a complete answer to another question posed in [BG].