In this study, biocompatible memristive devices utilizing peptide templated gold nanoparticles (AuNPs) have been fabricated. The memristive devices exhibit great performance e. g., high switching on-off ratio (> 10 6 ), ultra-low switching voltage (< 0.4 V), and reproducible resistive switching. The internal mechanism based on conductive filaments has been studied in depth. Modulation of voltage pulse signals imitated the synaptic behaviors of paired-pulse facilitation (PPF), spike-timing-dependent plasticity (STDP), and the transition from short-term plasticity (STP) to long-term plasticity (LTP). These results demonstrate that memristive devices based on peptide-templated AuNPs have promising prospects in non-volatile memory and brain-inspired applications.