This study presents the development of luminol and gold nanoparticle co-functionalized graphene oxide (GO-AuNPs-L) hybrids as enhanced luminogenic signaling molecules in the chemiluminescence immunoassay (CLIA) for detecting C-reactive protein (CRP), a key biomarker of inflammation and cardiovascular diseases. When compared to free luminol, the GO-AuNPs-L hybrids significantly increased and prolonged the CL signal based on their synergistic enhancement in electron transfer during CL production. Based on the performance, the hybrids were employed as signaling molecules in both well plate-based and lateral flow CLIA platforms, showing substantial improvements in signal intensity and sensitivity in CRP detection. These results highlight the potential of GO-AuNPs-L hybrids as versatile and highly sensitive luminogenic molecules for immunological CRP detection, offering promising applications in clinical laboratory settings as well as in point-of-care diagnostics.