Calcium silicate particles containing mesoporous SiO2 (CaSiO3@SiO2) on the surface were grafted onto polypropylene nonwoven. The PP nonwoven grafted CaSiO3 containing mesoporous SiO2 (PP-g-CaSiO3@SiO2) was characterized by TEM and TG. The adsorption behaviors of bisphenol A (BPA) on PP-g-CaSiO3@SiO2 were investigated. The results indicated that the large surface area and the SiOH groups of the material improved the adsorption capacities and affinity for BPA. The adsorption rate was fast, and the adsorption capacity was high, even with the background organic compound alginate sodium. The adsorption mechanism of BPA by PP-g-CaSiO3@SiO2 was investigated. Isothermal titration calorimetry (ITC) was used to illustrate the driving force for the adsorption of BPA. PP-g-CaSiO3@SiO2 was prepared simply without using any organic solvent and could be recycled and reused.