To any connected and simply connected nilpotent Lie group N, one can associate its group of affine transformations Aff(N). In this paper, we study simply transitive actions of a given nilpotent Lie group G on another nilpotent Lie group N, via such affine transformations. We succeed in translating the existence question of such a simply transitive affine action to a corresponding question on the Lie algebra level. As an example of the possible use of this translation, we then consider the case where dim(G)=dim(N) less than 6. Finally, we specialize to the case of abelian simply transitive affine actions on a given connected and simply connected nilpotent Lie group. It turns out that such a simply transitive abelian affine action on N corresponds to a particular Lie compatible bilinear product on the Lie algebra of N, which we call an LR-structure.