Recently developed needleless electrospinning and electrolithography are two successful techniques that have been utilized extensively for low-cost, scalable, and continuous nano-fabrication. Rational understanding of the electrohydrodynamic principles underneath these nano-manufacturing methods is crucial to fabrication of continuous nanofibers and patterned thin films. This research project is to formulate robust, high-efficiency finite-difference Fourier spectral methods to simulate the electrohydrodynamic evolution of thin polymer films. Two thin-film models were considered and refined. The first was based on reduced lubrication theory; the second further took into account the effect of solvent drying and dewetting of the substrate. Fast Fourier Transform (FFT) based spectral method was integrated into the finite-difference algorithms for fast, accurately solving the governing nonlinear partial differential equations. The present methods have been used to examine the dependencies of the evolving surface features of the thin films upon the model parameters. The present study can be used for fast, controllable nanofabrication.