In this study, gold nanoparticles (GNP) were stabilized for the first time as dimers by a conducting polymer (CP). The morphology of kissing particles was examined by high-resolution transmission electronic microscopy (HRTEM). The broad-band localized surface plasmon resonance (LSPR) tunable by solvent variation and molecular binding was demonstrated by UV-vis measurement. The sensitivity of the longitudinal LSPR to the surrounding media or the binding of a biomolecule was 6 times higher than that of the transversal LSPR. A homogeneous bioassay was directly developed from the highly stable GNP-CP dimers with LSPR as prober, and protein sensing with detection limit well below 100 ng/mL was achieved.