The present investigation represents the synthesis of new p-sulphonatocalix[8]arene-based silica resin, p-SC8SR (5) and its application for the enhanced removal of methylene blue (MB) dye from contaminated water. The new p-SC8SR (5) resin was characterized by FT-IR, SEM, and EDX spectroscopy. The adsorption of MB on p-SC8SR (5) was investigated systematically by evaluating the effects of adsorbent dosage, initial pH, contact time, dye concentration, and ionic strength. Excellent adsorption (94%) of MB on p-SC8SR (5) was achieved at pH 9.5, contact time 10 min by using 0.2 mol L-1 ionic strength and 2 x 10(-5) M initial MB dye concentration. Kinetic behavior of MB dye adsorption process on the newly synthesized p-SC8SR (5) adsorbent follows the pseudo-second-order rate model (R-2 = 0.998 and 0.999 for 2 x 10(-5) M and 1 x 10(-4) M, respectively). Adsorption isotherms were fitted well by the Freundlich model with excellent value of coefficient of determination (R-2) = 0.995 which demonstrated that the adsorption of MB follows multilayer mechanism. Wastewater samples contaminated with MB were used to assess efficiency of the p-SC8SR (5) adsorbent. Results indicated that newly synthesized p-SC8SR (5) was found to be efficient adsorbent. During the removal process, the role of different functional groups' cyclic structure was scrutinized and found that the ionic property as well as pi-pi interaction of host molecules played imperative role in the extent of adsorption.