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This paper designs a new multilayered particle anisotropic conductive film (ACF) compound. Using the particle-reinforced composite model and probability theory, the novel ACF compound is compared with three traditional ACFs having the same particle volume fraction. The particle-reinforced model applies the concept of bonded and debonded structures in the interfaces between the adhesive resin and the particles. The elastic modulus of the particle-reinforced ACF is a function of the particle volume fraction and the bonded condition. In the failure model, probability theory is used to calculate the probability of opening and bridging. The volume fraction of the conductive particles plays an important role in determining the optimal ACF design. The current results indicate that the flip chip packaging performed using the novel multilayered particle ACF compound (particles distributed in the top/bottom surface layers) exhibits superior particle-reinforcement properties and a lower failure probability than traditional ACFs. The improved understanding of reinforcement mechanisms and failure probability developed by this study facilitates the enhanced design of novel ACF compounds.