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Exploiting the multiple properties of nanozymes for the multimode lateral flow assay (LFA) is urgently required to improve the accuracy and versatility. Herein, we developed a novel plasmonic Au nanostar@PtOs nanocluster (Au@PtOs) as a multimode signal tag for LFA detection. Based on the PtOs bimetallic nanocluster doping strategy, Au@PtOs can indicate both excellent SERS enhancement and nanozyme catalytic activity. Meanwhile, Au@PtOs displays a better photothermal effect than that of Au nanostars. Therefore, catalytic colorimetric/SERS/temperature three-mode signals can be read out based on the Au@PtOs nanocomposite. The Au@PtOs was combined with LFA and applied for breast cancer exosome detection. The detection limit for the colorimetric/SERS/temperature mode was 2.6 × 103/4.1 × 101/4.6 × 102exosomes/μL, respectively, which was much superior to the common Au nanoparticles LFA (∼105exosomes/μL). Moreover, based on the fingerprint molecular recognition ability of the SERS mode, exosome phenotypes derived from different breast cancer cell lines can be discriminated easily. Based on the convenient visual colorimetric mode and sensitive SERS/temperature quantitative modes, Au@PtOs driven LFA can satisfy the requirements of accurate and flexible multimodal sensing in different application scenarios.