Green geopolymer/alginate hybrid spheres (GAS) were fabricated by a one-pot method. The hybrid spheres contained a honeycomb structure with plenty of functional groups. 99% Cu(II) in a 50 mg/L solution was removed with a dosage of 0.15 g/100 mL GAS. GAS was packed in a column for continuous removal of Cu(II) from water. This provides a new approach to fabricate green hybrid adsorbent.