massive data. Memristive devices (i.e., memristors) have a huge potential for developing novel highly efficient braininspired computing system, [1-7] which is considered as a promising candidate to replace the present computing system. Memristor exhibits excellent properties, e.g., simple structure, [8] multiple resistance states, [9] fast switching speed, [10] and good scalability, [11] which are very beneficial as the building block of future braininspired systems. Physical mechanism of memristor has been widely studied and the resistance change is mainly attributed to the formation and dissolution of filaments in the resistance-switching layer between two metal electrodes. [12] Recently, organic polymer materials as the resistance-switching layers of memristive devices have been reported, [13-16] with excellent memory properties of large switching ratio, [17] low operating voltage, [18] low cost, [19] and mechanical flexibility. [20] However, the organic memristive devices usually encounter rigorous issues of low stability due to the uncertain redox properties within organic polymer materials. [14,19] On the other hand, polymers with the typical donor-acceptor (D-A) type can adjust their microstructure to boost inner ion migration, [21-24] which plays an important role in the formation of conductive filaments of memristive devices. It has been reported that metal-containing polymers [25-34] actually belong To realize brain-inspired devices and systems, memristor is one of the significant alternatives in breaking through the infrastructure restrictions of present logic and memory devices. Organic materials have become popular to fabricate memristive devices due to their unique properties of low cost, mechanical flexibility, and compatibility with complementary metal-oxidesemiconductor technology. Metallopolymer is a new kind of promising organic materials functioning as the resistive-switching layers of memristive devices due to the unique donor-acceptor type structure, which performs good ability of tuning electron concentration to boost the migration of inner ions. Herein, a new metallopolymer MP1 containing ferrocene and triphenylamine is designed and synthesized, which is utilized as a resistiveswitching layer of memristor with active and inert electrodes of Ag and Pt, respectively. Process flow of devices is fully developed and MP1 is found to act as metal-ions-accommodation site with the great potential to boost the formation of conductive filaments in the active region. More interestingly, the conductance of Ag/MP1/Pt memristor can be modulated under various voltage pulses exhibiting distinguished electrical properties. Additionally, synaptic functions are successfully emulated using such MP1-based memristors. This work will greatly expand the further development of organic memristors for flexible brain-inspired systems.