The simultaneous capture and detection of biomolecules is crucial for revolutionizing bioanalytical platforms in terms of portability, response time and cost‐efficiency. Herein, we demonstrate how the sensitivity to external stimuli and changes in the local electronic environment of silver clusters lead to an advantageous biosensing platform based on the fluorometric response of bioactive luminescent silver clusters (BioLuSiC) confined in faujasite X zeolites functionalized with antibodies. The photoluminescence response of BioLuSiC was enhanced upon immunocomplex formation, empowering a wash‐free and quick biodetection system offering optimal results from 5 min. Proteins and pathogens (immunoglobulin G and Escherichia coli) were targeted to demonstrate the biosensing performance of BioLuSiC, and a human serum titration assay was also established. BioLuSiC will pave the way for innovative bioanalytical platforms, including real‐time monitoring systems, point‐of‐care devices and bioimaging techniques. Antibody‐functionalized zeolites embedding photoluminescent silver clusters offer simultaneous capture and detection of biomolecules since immunocomplex formation triggers fluorometric enhancement in the explored biohybrid. This simple biosensing concept will open the way to innovative miniaturized and portable bioanalytical platforms.