When metal nanoparticles are functionalized with charged ligands, the movement of counterions and conduction electrons is coupled, which enables us to develop electronic devices, including diodes, transistors, and logic gates, but dynamically modulating the conductivity of a synaptic device within these materials has proved challenging. Here we show that an artificial synapse can be created from thin films of functionalized metal nanoparticles using an active silver electrode. The electric-field-injected Ag + coordinates with carboxyl ligands that sets up a conduction bridge to increase the nanoparticle conductivity by reducing the electron tunneling/hopping energy barriers. The dynamic modulation of conductivity allows us to implement several important synaptic functions such as potentiation/depression, paired-pulse facilitation, learning behaviors including short-term to long-term memory transition, self-learning, and massed leaning vs spaced learning. Finally, based on the nonvolatile characteristics, the metal nanoparticle synapse is used to build a single-layer hardware spiking neural network (SNN) for pattern recognition.