The feasibility of using tea waste (TW) as a low-cost adsorbent for the adsorption of an anionic dye (Congo red) from aqueous solution has been investigated. Adsorption in a batch process was conducted to study the effect of adsorbent dosage, initial dye concentration, contact time, pH, and temperature. The experimental data were analyzed by the Langmuir, Freundlich, and Temkin models. The adsorption system was best described by the Langmuir isotherm (R-2 > 0.99). Adsorption kinetics followed a pseudo-second-order model (R-2 > 0.99). The effect of mechanical treatment (vibratory mill) was also studied. The experimental results showed that using this physical treatment leads to an increase in the adsorption capacity of TW from 32.26 to 43.48 mg/g. Thermodynamic analyses revealed that the adsorption of Congo red on TW was endothermic and spontaneous in nature. The results indicated that TW can be employed as a potential low-cost adsorbent for the removal of Congo red from aqueous solution.