Acute　myocardial　infarction　(AMI)　survivors　face　a　high　risk　of　mortality　as　a　result　of　increasing　heart　failure　and　irreparable　myocardial　injury.　New　portable　methods　for　immediate　diagnosis　must　be　developed　to　provide　patients　with　daily　warnings.　Herein,　the　development　of　a　dual-mode　photothermal-pyroelectric　output　system　based　on　a　point-of-care　platform　for　rapid　AMI　detection　is　reported.　Termed　as　Integrated　Photothermal-Pyroelectric　Biosensor　for　AMI　(IPPBA),　the　method　leverages　cascade　enzymatic　amplification　to　convert　the　target　signal　into　a　thermal　and　pyrooelectric　conversion　of　the　testing　process　by　delicate　pyroelectric　pervokite　NaNbO3　nanocubes　modified　microelectrodes　for　sensitive　detection　of　cTnI　protein　in　whole　blood.　In　addition,　the　mechanism　of　the　proposed　pyroelectric　bioassay　model　is　explored　in　depth　based　on　in　situ　variable　temperature　X-ray　diffraction　(XRD)　lattice　change　statistics　and　density　function　theory　(DFT)　calculations.　With　standard　samples　and　under　optimized　experimental　conditions,　the　proposed　IPPBA　platform　exhibits　excellent　signal　stability　and　ultra-low　detection　limit　(0.05 ng　mL–1)　for　the　target　cTn　I.　With　further　developments　in　digital　technology　(e.g.,　5G　signaling　protocols,　fully　automated　systems),　the　integrated　digital　bio-testing　platform　IPPBA　is　fully　capable　of　accomplishing　positive　and　timely　diagnosis　of　AMI.　©　2022　Wiley-VCH　GmbH.