Bioorthogonal catalysis can regulate the intracellular chemistry without the hindrance of the autoregulation for the homeostasis. However, complex intracellular environment and catalyst instability are big obstacles for the synthetic catalytic system not only to perform their functions inside cells, but also to regulate the catalysis like enzymes. We have fabricated the protein-sized biorthogonal nanozymes that can be regulated the intracellular catalysis. These nanozymes are consist of the water-soluble nanoparticles bearing the hydrophobic transition metal catalysts in their ligand shell and gate-keeping units using host-guest chemistry between the nanoparticle and cucurbit[7]uril. Their regulation mechanism design was from the allosteric regulation of enzymes. The intracellular catalytic systems were used for imaging and therapeutic applications through triggered cleavage of allylcarbamates for pro-fluorophore activation and propargyl groups for prodrug activation, demonstrating as a novel platform of the enzyme mimicking nanobot.