Biomolecule-functionalized Au nanoclusters (AuNCs) have drawn great interest in the electrochemiluminescence (ECL) field due to their unique optical/electrical properties, biocompatibility, and versatile bioapplication potentials. Herein, we proposed a two-in-one ECL probe of immunoglobulin G-encapsulated AuNCs (IgG-AuNCs) for the development of a high-performance ECL immunoassay (ECLIA) platform. The IgG-AuNCs were not only used as an ECL probe due to their excellent anodic ECL performance with triethylamine (TEA) as a coreactant but also used as the biorecognition element because of their well-retained bioactivity of the IgG. As a proof of concept, a new type of competitive immunosensing platform has been applied to detect IgG representing several merits of facile preparation, rapid detection, sample saving, and good analytical performance. The sensing platform exhibited a linear range of 0.5-50,000 ng/mL with a limit of detection of 0.06 ng/mL for IgG detection with high selectivity. In addition, this convenient ECLIA platform also performed well in real serum sample detection. Notably, our work not only proved the "two-in-one" immuno-AuNC probe-based ECLIA strategy but also developed a rational framework for study of ECL bioassay platforms based on multifunctional AuNCs and other related nanomaterials.