Quantitative fluorescence immunoassay is a vital and convenient method in point-of-care (POC) testing for food safety and clinical healthcare. However, current marking materials, from organic luciferin to quantum dots, still lack the requirement of increasing need for multiple targets of interest because of their too broad emission. Here, a new label material, perovskite nanocrystals (Pe-NCs), with a narrower photoluminescence spectrum is reported, and a sensitive and quantitative immunoassay method named the perovskite nanocrystal fluorescence-linked immunosorbent assay is preliminarily demonstrated. The key point of realizing water-dispersed and stable Pe-NCs was addressed by functionalizing with hydroxyl groups. The fluorescent probes (perovskite antibody) were constructed via electrostatic adsorption with narrow full-width at half-maximum (∼18 nm), laying the foundation for future study of multi-target detection. Both indirect competitive immunity and sandwich immunoassay were successfully demonstrated. This work provides a possible label material for POC tests and may open up a promising avenue of next-generation immunoassay.