The surface modification of Zeolite 4A using cetyl trimethyl ammonium bromide (CTAB) as a modifier via an ultrasonic method was carried out and the surface physicochemical properties measured. Response surface methodology (RSM) was developed with CTAB concentration, handling time, and handling temperature as variables, to help predict the performance of the modified zeolite under particular conditions. The influence of organic-modified surface treatment and of the amount of modified zeolite on the water-absorption capability of starch-g-poly (acrylic acid) hydrogel composites was also assessed. The results showed that the channels and skeleton structure of zeolite 4A were unchanged after organic modification by CTAB and the surface modification was effective. The results suggest that organic-modified zeolite 4A has improved the water-absorption capability.