This paper contains a large set of spectra of low-redshift, radio-loud quasars at low resolution (20-25 angstrom). The spectral range covers most of the important optical spectral lines, ranging from H-alpha 6562 angstrom in some objects to [Ne v] 3426 angstrom in others. The sample has the advantage of being observed and reduced in a uniform manner, as well as being considerably larger than previous surveys of radio-loud quasars. In this paper we discuss the observations and analysis and present the spectra. In Paper II we discuss the results.