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Polytetrafluoroethylene/aluminum (PTFE/Al) reactive material is a pivotal research object in the aerospace, military, and mechanical engineering fields and can release chemical energy (CE) under shock or impact. However, its relatively low mechanical strength limits its applications. The present paper proposes a Cu-PTFE/Al (73.5wt. %/26.5wt. %) double-layer liner that can form tandem explosive formed projectiles (EFPs) under the shock of shaped charges, which not only retains the strong penetration ability but also shows a more significant lateral enhancement effect through the deflagration reaction. Here, the preparation process of the PTFE/Al liner is given, and an analytical model for the Cu-PTFE/Al tandem EFP of the damage process against multi-spaced plates is established, revealing the penetration and deflagration-enhanced mechanisms. Subsequently, a two-step segmented numerical simulation for the penetration–deflagration coupling effects is conducted, and the time-space interaction process and damage results between kinetic energy penetration and CE deflagration are obtained. A series of experiments of tandem EFPs against spaced plates are conducted, including the different materials, thickness ratio, and standoff. Experimental results show that compared with Cu–Cu tandem EFP with the same condition, the penetration ability of Cu-PTFE/Al composite EFP is reduced, but the damage enhancement effect is greatly improved; the maximum damage area of a single plate is increased by 220.1%, and the average damage area of a single plate is increased by 76.2%. This study provides important reference data and a theoretical basis for the design of metal-reactive tandem EFPs. [ABSTRACT FROM AUTHOR]