Holarrhena antidysenterica (Ha) and Citrullus colocynthis (Cc) biowaste from indigenous Pakistan resources was used to remove toxic brilliant green (BG) dye from aqueous solutions in a batch mode. Tartaric acid chemical modification gave promising results than the nonmodified forms of biowaste. Surface characterization was carried out by FT-IR and SEM. The optimum conditions for (BG) dye elimination by Ha-tartaric acid modified (Ha-Ta) were 1.8 g, 45 minutes, 4.0 pH; 40°C, and 100 rpm and with Cc-tartaric acid modified (Cc-Ta) were 1.6 g, 45 minutes, 6.0 pH; 40°C, and 150 rpm dye solution shaking rate, which gave optimum results. Equilibrium data of raw and chemically modified biowaste followed the Langmuir model indicating monolayer chemisorption. Qmax values were found to be 55.24 mg/g, 112.35 mg/g, 50.50 mg/g, and 79.36 mg/g for Ha, Ha-Ta, Cc, and Cc-Ta. Kinetics followed the pseudo-second-order kinetic model. Dye removal involved surface and intraparticle mode of diffusion. Thermodynamic studies proved the process to be spontaneous and exothermic one. The adsorbents can be effectively utilized for the removal of toxic basic dyes, such as BG from wastewaters.