In the present study, safe, efficient and multifunctional 3D GO based polymeric gels were prepared by the promotion of different biopolymer agents. The obtained freeze-dried 3D gels have a well-defined and interconnected 3D porous network, which allows the adsorbate molecules to diffuse easily into the adsorbent. AFM images confirmed that the biopolymers had been successfully adsorbed onto the GO nanosheets through noncovalent interactions with apparently increased thicknesses. In this proposed biologically 3D noncovalent assembly, the use of biopolymers, such as proteins, DNA, and chitosan, plays an essential role in the advancement of biologically compatible adsorbents and the realization of novel, multifunctional and heterogeneous integration of materials. Meanwhile, the blood compatibility of the GO/biopolymer gels was investigated by using human red blood cells (RBCs), which indicated that the as-prepared GO/biopolymer gels exhibited ultralow hemolysis ratio (lower than 1%) and better RBCs compatibility than the pristine GO sponge, since the adsorbed biopolymers could effectively mediate the surfactant-like property of the GO sheet. Furthermore, the 3D GO/biopolymer gels revealed ultra-high adsorption capacities against toxic cationic molecules and heavy metal ions, and presented great potential in blood purification fields. Moreover, the obtained gels also presented multifunctional ability, e.g. drug molecule delivery, and had high drug loading capacity and controllable releasing speed. The excellent blood compatibility and high toxic molecules loading capacity of the GO/biopolymer gels might confer it great potentials for various blood-contact applications.