In this study, zeolitic materials were synthesized from Jeju Volcanic Rocks (JVR) using a fusion/hydrothermal method at NaOH/JVR ratios of 0.6 and 1.2. The crystallinities of the zeolitic materials at NaOH/JVR ratios of 0.6 and 1.2 were 25.5% and 59.0%, respectively. It was confirmed through the SEM image that the zeolitic materials covered the zeolite particle with a cube-shaped crystals. The Co ions adsorption by the zeolitic materials were to reach the adsorption equilibrium at 120 min. It could be better simulated in the pseudo-second order adsorption kinetic equation than in the pseudo-first order adsorption kinetic equation. The adsorption capacities (qm) of Co ions could be to estimate Langmuir isotherm better than Freundlich isotherm. The maximum adsorption capacities (qm) at NaOH/JVR ratios of 0.6 and 1.2 were 55.3 mg/g and 68.7 mg/g, respectively. It was found that there was a high correlation between the crystallinity of zeolitic materials and the adsorption capacity of Co ions adsorption.