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We have investigated the electrical properties of anisotropic conductive adhesive (ACA) joint using submicrometer-sized (~500 nm in diameter) silver (Ag) particle as conductive filler with the effect of π-conjugated self-assembled molecular wires. The ACAs with submicrometer-sized Ag particles have higher current carrying capability (~3400 mA) than those with micro-sized Au-coated polymer particles (~2000 mA) and Ag nanoparticles (~2500 mA). More importantly, by construction of π-conjugated self-assembled molecular wire junctions between conductive particles and integrated circuit (IC)/substrate, the electrical conductivity has increased by one order of magnitude and the current carrying capability of ACAs has improved by 600 mA. The crucial factors that govern the improved electrical properties are discussed based on the study of alignments and thermal stability of molecules on the submicrometer-sized Ag particle surface with surface-enhanced Raman spectroscopy (SERS), providing a fundamental understanding of conduction mechanism in ACA joints and guidelines for the formulation of high-performance ACAs in electronic packaging industry.