Well-ordered one-dimensional nanostructures are enabling important new applications in textiles, energy, environment and bioengineering owing to their unique and anisotropic properties. However, the production of highly aligned nanofibers in a large area remains a significant challenge. Here we report a powerful, yet economical approach that integrates the concepts of the parallel-electrode electrospinning with centrifugal dispersion to produce nanofibers with a high degree of alignment and uniformity at a large scale. We first demonstrated this approach with polyvinylidene fluoride to show how experimental parameters regulate fiber properties, and then with chitosan, a natural polymer, and polyethylene oxide, a synthetic polymer, to illustrate the versatility of the system. As a model application, we then demonstrated the significance of fiber alignment in improving the piezoelectric effect for voltage generation. The technique presented here may be used for mass production of aligned nanofibers of various polymers for a myriad of applications.