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This work focuses on an interdisciplinary issue in energy management and biosensing techniques. Aiming at enhancing the biosensing detection of dopamine at high ambient temperatures, we developed an innovative integration of phase-change microcapsules with a metal−organic framework (MOF) based on zeolitic imidazolate framework-8 to develop an intelligent electrochemical biosensing system with a thermal self-regulation function. We first fabricated a type of electroactive microcapsules containing a MOF-anchored polypyrrole/SiO 2 double-layered shell and a phase-change material (PCM) core. The resultant microcapsules not only exhibit a regular spherical morphology with a layer-by-layer core−shell microstructure but also display an effective temperature-regulation capability to enhance enzymatic bioactivity under phase-change enthalpies of around 124.0 J•g −1 along with good thermal impact resistance and excellent thermal cycling stability for long-term use in thermal energy management. These electroactive microcapsules were then used to modify a working electrode together with laccase as a biocatalyst to construct a thermal self-regulatory biosensor. With a high sensitivity of 3.541 μA•L•μmol −1 •cm −2 and a low detection limit of 0.0069 μmol•L −1 at 50 °C, this biosensor exhibits much better determination effectiveness toward dopamine at higher temperatures than conventional biosensors thanks to in situ thermal management derived from its PCM core in the electroactive microcapsules. This study offers a promising approach for development of intelligent thermal self-regulatory biosensors with an enhanced detection capability to identify various chemicals accurately in a wide range of applicable temperatures.