Two superstructures of {Cs[Ni(Hbim)(3)]}(n) (A) and {[Ni(Hbim)(3)](2) Cs((NPr4)-Pr-n). MeOH}(n) (B) were formed by a self-organization with [Ni(Hbim)(3)](-1) building blocks, which use both coordination geometry and three intermolecular sites of Hbim(-1). The networks of A and B have indicated 2-D honeycomb sheets and 3-D double-helical structure, respectively. Their formations are owed to the existence of a Cs+ ion due to a strong interaction with the [Ni(Hbim)(3)](-1).