In the pursuit of more secure information transfer, advanced nanoelectronic technologies and nanomaterials must be developed. Here, a material is presented able to undergo an unprecedented light-pumped directional charge-transfer process reminiscent of toppling dominoes. The material is based on ortho-fluorinated azobenzene molecules which are organized in molecular rows by the regular array of a metal–organic framework. The azobenzene molecules undergo light-induced trans→cis forward as well as electrocatalytic cis→trans backward isomerization. The findings reveal that electron hopping occurs in a sequential and propagating manner between the light-generated cis isomers along with an isomerization of the sample to the trans-state. Thus, light can be used to locally write information, which subsequently can be read out by the transferred charge with simultaneous deletion of the information. This freely repeatable, self-erasing domino information transfer is a groundbreaking new mechanism to process information on the molecular level that may find application in encryption.