Colloidal quantum dots (CQD) have emerged as attractive materials for infrared (IR) photodetector (PD) applications because of their tunable bandgaps and facile processing. Presently, zinc oxide is the electron‐transport layer (ETL) of choice in CQD PDs; however, ZnO relies on continuous ultraviolet (UV) illumination to remove adsorbed oxygen and maintain high external quantum efficiency (EQE), speed, and photocurrent. Here, it is shown that ZnO is dominated by electropositive crystal planes which favor excessive oxygen adsorption, and that this leads to a high density of trap states, an undesired shift in band alignment, and consequent poor performance. Over prolonged operation without UV exposure, oxygen accumulates at the electropositive planes, trapping holes and degrading performance. This problem is addressed by developing an electroneutral plane composition at the ZnO surface, aided by atomic layer deposition (ALD) as the means of materials processing. It is found that ALD ZnO has 10× lower binding energy for oxygen than does conventionally deposited ZnO. IR CQD PDs made with this ETL do not require UV activation to maintain low dark current and high EQE.