AbstractThe implementation of probabilistic algorithms by deterministic hardware is demanding and requires hundreds of instructions to generate a pseudo‐random sequence of numbers. On the contrary, the dynamics at the molecular scale is physically governed by probabilistic laws because of the stochastic nature of thermally activated and quantum processes. By simulating the exciton transfer dynamics in a multi‐chromophoric system, we demonstrate the implementation of a random walk that samples the possible pathways of a traveler through a network and can be probed by time‐resolved fluorescence spectroscopy. The ability of controlling the spatial arrangement of the chromophores allows us to design the “landscape” in which the traveler is moving and therefore to program the molecular device.