Using low-cost and naturally available materials is considered an optimal adsorbent for removing phosphorus (P) from water due to its simplicity and economic efficiency. This study examined the removal of P from water using volcanic ash soil (VAS) by batch and column experiments. The maximum adsorption capacity of P was 2.94 mg g−1, estimated from the batch experiment according to a Langmuir isotherm. The column study showed a higher adsorption capacity of 5.57 mg g−1. The breakthrough curve showed that influent water containing 2 mg L−1 P was completely purified by VAS within 1,230 pore volumes (PV). The breakthrough and saturation points of the curves were 3,100 PV and 14,875 PV, respectively. After an adsorption column was loaded with 20,508 PV, a regeneration procedure was developed to determine whether an ion exchange of P with chloride occurred or adsorbed P in the columns could be eluted. Approximately 20% of P was recovered from columns by desorption tests, regardless of NaCl solution or deionized water. Specific surface area and mineral concentrations are both important characteristics that improve the adsorption capacity of VAS. The present study suggests that VAS is a promising adsorbent to remove P in water.