Fukushima Dai-ichi Nuclear Power Plant (FDNPP) accident produced much amount of radioactively contaminated water at the Great East Japan Earthquake. 137Cs and 90Sr have been focused to remove from the contaminated water using zeolite types of adsorbents. Other radionuclides have been treated and removed separately by Advanced Liquid Processing System (ALPS), where resin is used to immobilize anions. However, these kinds of spent-adsorbents are not suitable for long-terms burying because of its instability, and the representative anionic radionuclides (129I, 36Cl, 99mTc and 79Se) have quite long half-life (105-107 years). Montmorillonite (Mt) is an useful adsorbent because of its high chemical stability and large cationic exchange capacity. In the present work, surfactant modified Mt (OMt) has been developed using hexadecylpyridium chloride for adsorption of ClO4-, which is a surrogate of 99mTcO4-. For stabilization of spent-OMt, cement solidification was examined with varying the ratio of spent-OMt content. To evaluate its chemical and physical stability, soaking and compressive strength tests were conducted. As a result, it was revealed by FTIR and 29Si-NMR that with increase in OMt contents, the linkage of calcium silicate hydrate was more developed.