Ion adsorption by fungal hyphae (FH)-supported adsorbents represents a promising approach to remove the radioactive ion in water, whereas the existing organics in wastewater reduce the adsorption efficiency. Herein, we developed FH-graphene-MoS2 hybrid nanosheets which enabled efficient adsorption of radioactive ions through the photodegration of organics. In the hybrid material, graphene nanosheets coated FH nanoframes with considerable surface area serves as adsorption agent, together with the deposited MoS2 nanosheets as photo-degradation material. Moreover, photoelectrons produced by MoS2 further promoted the adsorption ability by reducing the U(VI) to U(IV). In the treatment of wastewater which contains U(VI) and tannic acid (TA) under irradiation, the MoS2 in FH-graphene-MoS2 hybrid nanosheets decomposed TA and thus reduces the occupation of adsorption sites, which greatly promoted the adsorption capacity of FH-graphene hybrid nanosheets for U(VI).