Nickel-based magnetic activated carbon was synthesized from coconut shell activated carbon by electroless plating with palladium-free activation. The effect of plating solution volume on metallic ratio and adsorption capacity were evaluated. The effect of metallic ratio on specific area, pore volume, and magnetic properties were investigated. The morphologies of activated carbon before and after plating were observed by SEM, and the composition of the layer was analyzed by EDS analysis. The results showed that the metallic ratio was increased with the increase of the plating solution volume. The magnetic activated carbon showed high adsorption capacity for methylene blue and a high iodine number. Those values reached 142.5 mg/g and 1035 mg/g, respectively. The specific area and pore volume decreased from 943 m2/g to 859 m2/g and 0.462 ml/g to 0.417 ml/g, respectively. And the layer was more compact and continuous when the metallic ratio reached 16.37 wt.%. In the layer, there was about 97 wt.% nickel and 3 wt.% phosphorus, which indicates that the layer was a low-phosphorus one. At the same time, magnetism was enhanced, making the product suitable for some special applications.