It is shown that the performance of photoelectrochemical cells based on the lamellar material InSe can be considerably improved by means of a selective (photo)electrochemical etching. Whereas the cleavage Van de Waals plane (⊥ tocaxis) shows little improvement, the photcurrent in the ∥ face (parallel to thecaxis) is doubled (30 mA cm−2under AM1 illumination). Forn‐type InSe a reverse bias (+1.5 V versus standard calomel electrode SCE) was employed during the photoetching,p‐InSe electrodes were electrochemically etched by applying a forward bias (+1.5 V). In both cases, surface holes carry out the selective corrosion of the semiconductor surface which is another manifestation for the asymmetry played by holes and electrons on semiconductor surfaces. It is hoped that this finding will pave the way for the construction of high‐efficiency solar cells based on a thin film made of lamellar materials.