The quasi-periodic optical superlattice is a promising material for use in optical frequency conversion. We propose a method for designing a quasi-periodic structure for efficient third-harmonic generation (THG) at any given wavelength. With this method we have made a LiTaO(3) sample in which 27% THG at 0.48microm was achieved, together with a series of highly efficient multiwavelength second-harmonic generation outputs. The result is in good agreement with the theoretical prediction.