Mixture of a number of enzymes for cascade catalysis has been broadly utilized in biomedicine, however integration of pure bioenzyme with inorganic nanozyme is much less developed. Impressed by the considerable content material of superoxide dismutase (SOD) in Spirulina platensis (SP), we set up built-in cascade catalysis for anti-inflammation remedy via adorning catalase (CAT)-biomimetic ceria nanoparticles (CeO2) onto SP floor through electrostatic interplay to construct microalgae-based biohybrids. The biohybrids reveals mixed catalytical competence for preferentially reworking superoxide anion radicals (O2•−) to hydrogen peroxide (H2O2), and subsequently catalyzing H2O2 disproportionation to water and oxygen. In ulcerative colitis and Crohn’s illness, the biohybrids reveals passable therapeutic impact owing to the synergistic reactive oxygen species (ROS)-scavenging capability, proposing new practice of thought for enzymes-based biomedical software.