In this work, poly(carboxybetaine methacrylate) hydrogel (pCBMA) was employed to modify the activated carbon (AC) for improving the biocompatibility and adsorption capacity of AC in biological environments. First, size-controlled hydrogel beads and hydrogel coated AC (pCBMA-AC) were fabricated with a homemade device, and the preparation conditions were optimized. Then the physical and biological properties of pCBMA-AC with different diameters were investigated. 2 mm pCBMA-AC dispalyed excellent stability with leakage rate only 0.16% after 72 h shaking incubation, as well as remarkable biocompatibility with merely 0.13% hemolysis rate and 3.41% cell death, while 14.72% and 70.11% for the bare AC, respectively, indicating the acceptable lower hemolysis and cytotoxicity according to ISO 10993. Furthermore, the adsorption capacities of pCBMA-AC were evaluated in biological environments with methylene blue as model molecules. The pCBMA-AC displayed 93.50% and 97.32% adsorption rates in BSA solution and FBS, respectively, but only 70.33% and 40.26% for the uncoated AC. These results indicated that pCBMA endows AC remarkable biocompatibility and adsorption capacity, which could extend the applications of AC in biological environments.