Acetylcholinesterase (AChE) plays a critical role in maintaining nervous system homeostasis and coordinating essential biological reactions. AChE is an important biomarker for early diagnosis and treatment, including Parkinson's disease (PD), Alzheimer's disease (AD), and Huntington's disease (HD). Therefore, developing efficient and immediate sensing platforms for AChE detection is crucial for advancing early diagnostic tools. In this study, we developed a dual-mode colorimetric/photothermal sensing platform based on iodide ion-synergized covalent porphyrin-triazine backbone nanozymes (Zn-CTF/I) to detect AChE with high sensitivity and reliability. The synergistic interaction between iodide ions and zinc atoms effectively modulated the electronic structure of the catalytic active site, significantly enhancing the peroxidase-like (POD-like) activity of Zn-CTF/I. This enhancement led to a 10-fold reduction in the AChE detection limit compared to controls, with a minimum detection limit of 0.003 U L, outperforming other reported assays. The integration of temperature-based photothermal signals with colorimetric detection improved the platform's accuracy and reliability. The system also demonstrated excellent recovery performance in detecting AChE in complex serum samples. The proposed dual-mode sensing platform provides a sensitive, reliable, and robust tool for AChE detection, with promising applications in early diagnosis and treatment monitoring of neurodegenerative diseases.