Dye wastewater causes serious health problems that may not be solved by traditional methods. The present study deals with the removal of methyl violate (MV), methyl green (MG), and methyl blue (MB) by highly efficient and regenerable calix[4]arene based impregnated material from aqueous media. The material was characterized by different analytical techniques. Both batch and column sorption methods were used and various parameters including pH, adsorbent dosage, initial concentration, equilibrium time, temperature, and electrolyte were optimized. The kinetic and thermodynamic parameters were also evaluated. The material was 99% effective to remove these dyes from real wastewater samples. Recovery of the material and dye was achieved with 5% HCl that signifies reusability of the material again and again.