We prove that a group $Γ$ admits a discrete topological (equivalently, smooth) action on some simply-connected 3-manifold if and only if $Γ$ has a Cayley complex embeddable -- with certain natural restrictions -- in one of the following four 3-manifolds: (i) $\mathbb{S}^3$, (ii) $\mathbb{R}^3$, (iii) $\mathbb{S}^2 \times \mathbb{R}$, (iv) the complement of a tame Cantor set in $\mathbb{S}^3$.