Advanced Enzyme Mimicking Engineering: 3D Biomimetic Pt Single‐Atom Nanozymes Initiating Pressure‐Driven Device

Abstract Current research on single‐atom nanozymes has predominantly concentrated on 2D structures, with limited exploration into the influence of 3D biomimetic structures on their catalytic performance. In this work, a 3D nanostructure of Pt single‐atom nanozyme (Pt‐NC SAzyme) is fabricated by encapsulating platinum 2,4‐pentanedionate in each molecular cage of ZIF‐8 and then pyrolyzing. X‐ray absorption fine structure analysis confirmed the presence of Pt as single atoms, with each Pt atom exclusively coordinated with four nitrogen atoms, while the *O is identified as an intermediate in the catalytic reaction. Additionally, theoretical calculations demonstrated that Pt‐NC SAzyme exhibited a lower potential energy and a shorter pathway for catalyzing the production of O 2 from H 2 O 2 than that of 2D Pt‐NC due to the localization effect, confirming a superior catalase‐like activity of Pt‐NC SAzyme. Based on the efficient O 2 production from Pt‐NC SAzyme, a dual‐mode pressure immunosensor is established to achieve sensitive detection of aminopyrine by converting gas‐induced pressure into visual and timing readouts. This work introduced a novel approach to enhance the catalytic activity of SAzymes through bionic structural design and coordination environment, while also proposing a new concept for point‐of‐care testing in food safety, environmental monitoring, and disease diagnosis.