For electrically conductive adhesives (ECAs), high electrical conductivity generally conflicts with excellent mechanical properties because electrical conductivity increases while desirable mechanical properties decrease with the increase in loading of conductive fillers or removal of lubricants on the silver filler surface. In this work, a method was developed to improve both the electrical conductivity and mechanical properties of the ECAs by introducing double bonds. Itaconic acid (IA) was used to replace the lubricant on the silver flake (Ag-F) surface, and acrylic acid (AA) was used as part of the ECA resin matrix. IA can replace the lubricant on the Ag-F surface, similar to other short-chain dibasic acids, to improve the ECA electrical conductivity. Furthermore, IA can be polymerized with AA to form covalent bonds between the silver flakes and the resin matrix, enhancing the mechanical properties of ECA. Compared with ECA filled with commercial silver flakes, the electrical conductivity of ECA filled with IA-treated silver flakes increased by ~ 21%, and the lap shear strength increased by ~ 29%.