Biolipid Film‐Fused Electrochemiluminescence for Multipurpose In Situ Bioassays

ABSTRACT Electrochemiluminescence (ECL) is intrinsically a surface‐state‐sensitive strategy, yet its seamless synergy with soft biomembranes remains sparsely explored. Herein, a biolipid‐bound, membrane‐interactive scaffold is built upon an ECL‐emissive artificial nanochannel and smoothly blended into supported phospholipid bilayers containing cholesterol and diversified natural or synthetic lipids. Such bilayer‐bridged assemblies preserve efficient emission while permitting dynamic membrane remodeling. The resulting biointerface enables label‐free profiling of cytomembrane‐active species, including divalent cations, amphiphilic pharmaceuticals, and pore‐forming peptides, through real‐time isotherm and kinetic analysis. By further integrating phospholipid‐pendant recognition motifs, femtomolar detection of Alzheimer's disease biomarkers (β‐amyloid polypeptide and tau protein) is achieved. Moreover, vesicle‐mediated membrane merging embeds ECL emitters into living‐cell plasmalemma, affording surface‐confined single‐cell visualization using endogenous oxygen as the coreactant. Collectively, this biointerface‐compatible ECL paradigm enables multiplexed monitoring of molecular, membranous, and cellular processes via membrane‐structural modulation.