In the current paper, a novel amphoteric straw-based adsorbent was prepared and applied to adsorb various dyes from aqueous solutions. The amphoteric adsorbent was proven effective in eliminating both cationic and anionic dyes (methylene blue and acid green 25), especially at corresponding favored pH conditions. The fundamental adsorption behavior of the adsorbent on removing various dyes was also investigated at different temperatures. The adsorption isotherms were all best-fitted by the Langmuir equation, whereas the adsorption kinetics was well-described by both the pseudo-second order model and the Elovich model. The experimental result revealed that the adsorption mechanism followed the monolayer chemical adsorption with an ion-exchange process.