The attenuation layer method has been considered an effective countermeasure to deal with excavated soils and rocks containing geogenic toxic elements like arsenic (As). The geosynthetic sorption sheet is a geosynthetic product that can be employed in the attenuation layer method applications as a sorption material. The sorption sheets used in the attenuation layer will be inevitably subjected to overburdened loads in the field. In this study, laboratory column experiments are conducted to evaluate the attenuation performance of the geosynthetic sorption sheets coated with hydrotalcite as sorbent against As under different overburden pressure conditions (10, 100, and 200 kPa). Experimental results showed that the cumulative sorption masses of As for 200 kPa cases are approximately 10.5–13.3 times greater than that for 10 kPa cases. Microstructure characterizations of the geosynthetic sorption sheet before and after loading were also detected. More compacted and involved fiber configuration as a result of higher loading produces a more effective contact between As solution and hydrotalcite. The presence of partial dissolution of hydrotalcite is confirmed through the chemical analysis of effluent. However, hydrotalcite would gradually become stable during continuous use.