Water is one of the most important resources for human survival and development. Efficient wastewater treatment techniques such as coagulation, filtration, ozonation, and reverse osmosis have been studied to remove toxic materials from water. Implementation of adsorption columns has been proven to be an efficient wastewater treatment method, particularly for the removal of organic contaminants. In this study, we present the preparation of an eco-friendly graphene oxide–chitosan (GC) composite hydrogel column (GCCHC) and its application as a broad-spectrum adsorbent for wastewater treatment. The GCCHC shows a high removal capacity towards different contaminants including both cationic dyes [methylene blue (MB) and rhodamine B (RhB)] and anionic dyes [methylene orange (MO) and congo red (CR)]. Moreover, the samples can be regenerated and recycled without loss of contaminant removal capacity over successive adsorption and washing cycles.