Biomolecular materials offer tremendous potential for the development of memristive devices due to their low cost of production, environmental friendliness, and, most notably, biocompatibility. Herein, biocompatible memristive devices based on amyloid-gold nanoparticle hybrids have been investigated. These memristors demonstrate excellent electrical performance, featuring an ultrahigh R off /R on ratio (>10 7 ), a low switching voltage (<0.8 V), and reliable reproducibility. Additionally, the reversible transition from threshold switching to resistive switching mode was achieved in this work. The arrangement of peptides in amyloid fibrils endows the surface polarity and phenylalanine packing, which provides channels for the migration of Ag ions in the memristors. By modulating voltage pulse signals, the study successfully imitates the synaptic behavior of excitatory postsynaptic current (EPSC), paired-pulse facilitation (PPF), and the transition from short-term plasticity (STP) to long-term plasticity (LTP). More interestingly, Boolean logic standard cells were designed and simulated using the memristive devices. The fundamental and experimental results of this study thus offer insights into the utilization of biomolecular materials for advanced memristive devices.