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Synaptic plasticity, the dynamic tuning of signal transmission strength between neurons, serves as a fundamental basis for memory and learning in biological organisms. This adaptive nature of synapses is considered one of the key features contributing to the superior energy efficiency of the brain. Here, we use molecular dynamics simulations to demonstrate synaptic-like plasticity in a subnanoporous two-dimensional membrane. We show that a train of voltage spikes dynamically modifies the membrane’s ionic permeability in a process involving competitive bicationic transport. This process is shown to be repeatable after a given resting period. Because of a combination of subnanometer pore size and the atomic thinness of the membrane, this system exhibits energy dissipation of 0.1 to 100 aJ per voltage spike, which is several orders of magnitude lower than 0.1 to 10 fJ per spike in the human synapse. We reveal the underlying physical mechanisms at molecular detail and investigate the local energetics underlying this apparent synaptic-like behavior.