Provided are modified coffee and/or cacao, and/or coffee-substitute and/or cacao/chocolate-substitute compositions, and methods of making same, comprising cross-Maillardized substrate carrier materials (e.g., plant materials, etc.), or non-cross-Maillardized carrier materials, having cross-Maillardized reaction products providing for improved and/or more organoleptically accurate coffee-substitute or cacao/chocolate-substitute compositions. These coffee or cacao/chocolate, and/or coffee-substitute and/or ca-cao/chocolate-substitute compositions, comprise extracts, kernels, grounds, powders beverages, concentrates, flavorings, etc., based thereon, with or preferably without coffee or cacao beans. The methods comprise contacting a substrate carrier material, having endogenous Maillard-reactive nitrogen and/or carbohydrate constituents, with an exogenous Maillard reagent comprising exogenous Mail-lard-reactive nitrogen and/or carbohydrate constituents, wherein the exogenous Maillard reagent comprises elevated levels of e.g., leucine, to provide conditioned substrate carrier materials, for reacting to produce cross-Maillardized products. Cross-Maillard-primed substrate carrier materials, are provided, along with regenerated spent coffee and non-coffee grounds. Modified cocoa, chocolate and/or chocolate-substitute compositions (e.g., bars, chips, etc.) are also provided.