Chili stalk powder (CS), a non-conventional adsorbent, has been exercised for facile removal of cationic dyes from simulated and wastewater by batch technique. The prepared material has been characterized by Fourier-transform infrared spectroscopy (FTIR), Field emission scanning electron microscopy (FESEM), Brunauer-Emmett-Teller analysis (BET), powder X-ray diffraction (powder XRD), and pHZPC and tested best with methylene blue and crystal violet under ambient conditions. FTIR denotes the presence of carbonyl and polyphenolic groups, responsible for dye adsorption. BET surface area analysis evaluates the porous nature and specific surface area of the material, and powder XRD confirms its amorphous nature. The porous structure could be ascertained from the FESEM image, and energy dispersive X-ray analysis (EDX) confirms the elemental composition. The pH above pHzpc shows an increase in removal efficiency. The maximum adsorption capacities are 49.53 and 36.88mg/g for methylene blue (MB) and crystal violet (CV) respectively. Linear as well as non-linear plots for kinetic and isotherm models were studied. Both dye uptake fits the linear plot of Langmuir adsorption isotherm (R2 = 0.999 and 0.995) and pseudo-second-order kinetics (R2 = 0.998 and 0.999). In the non-linear plot, the adsorption process for both dyes fit Langmuir (R2 = 0.999 for MB and R2 = 0.983 for CV) as well as Freundlich adsorption (R2 = 0.999 for MB and R2 = 0.994 for CV). 75.48% crystal violet (CV) and 73.35% methylene blue (MB) regeneration were successful in 1:1 methanol medium and reused for up to three cycles. The uptake mechanism is suggested to be a union of π-π stacking, electrostatic interaction, and weak hydrogen bonding. The material was tested with industrial effluent to prove its application in real wastewater treatment. Moreover, the material shows superior adsorption capacity than contemporary phytosorbents. To conclude, a zero-cost adsorbent using green chili stalk has been demonstrated for wastewater treatment.