The present invention comprises methods for making compositions derived from Ilex species, particularly Ilex paraguariensis, having lowered caffeine and tannin concentrations, compositions made by such methods, oral delivery formulations, and methods of use of such compositions. In particular, the present invention comprises methods for making mate compositions that have a predetermined characeteristic, such as a lowered amount of caffeine, elevated amounts of caffeoyls, and/or lowered amounts of tannin compounds compared to the native mate plant materials. Further, the invention comprises methods of additional processing steps to produce compositions having a predetermined alkaloid ratio or profiles to meet particular considerations for final products. The compositions of the present invention may be processed for specific uses such as tablets or other oral delivery vehicles. These compositions may be used in methods for treatment of physiological and medical conditions.