A structure of electrical-luminescent bifunctional bistrand-aligned nanobundles has been successfully fabricated by specially designed parallel spinnerets electrospinning technology. Eu(BA)(3)phen (BA = benzoic acid, phen = 1,10-phenanthroline) and polyaniline (PANI) were respectively incorporated into polyvinyl pyrrolidone (PVP) and electrospun into bistrand-aligned nanobundles with PANI/PVP as one strand nanofiber and Eu(BA)(3)phen/PVP as another strand nanofiber. The morphologies and properties of the final products were investigated in detail by scanning electron microscopy, transmission electron microscopy, fluorescence spectroscopy, Hall effect measurement system, and UV-Vis-NIR spectrophotometer. It is found that the as-prepared samples exhibit the nanostructures of bistrand-aligned nanobundles. The mean diameter for individual nanofiber of the bistrand-aligned nanobundles is 180 nm. The [PANI/PVP]//[Eu(BA)(3)phen/PVP] bistrand-aligned nanobundles possess excellent electrical conduction and luminescent properties. Fluorescence emission peaks of Eu3+ are observed in the [PANI/PVP]//[Eu(BA)(3)phen/PVP] electrical-luminescent bifunctional bistrand-aligned nanobundles and assigned to D-5(0) -> F-7(0) (581 nm), D-5(0) -> F-7(1) (592 nm), D-5(0) -> F-7(2) (615 nm) energy levels transitions of Eu3+ ions, and the D-5(0) -> F-7(2) hypersensitive transition at 615 nm is the predominant emission peak. The electrical conductivity reaches up to the order of 10(-3) S/cm. The electrical conductivity and luminescent intensity of the bistrand-aligned nanobundles can be tunable by adding various amounts of PANI and rare earth complex. The novel [PANI/PVP]//[Eu(BA)(3)phen/PVP] electrical-luminescent bifunctional bistrand-aligned nanobundles have potential applications in display devices and nanomechanics, etc. owing to their excellent electrical conduction and fluorescence.