Polychlorinated biphenyls (PCB) are synthetic organochlorine compounds with potential neurotoxic effects. Although negative effects on neuropsychological development have been observed in previous studies on PCB exposure, there are inconsistencies in these effects at current exposure levels of these compounds which are much lower than for previous generations. This study aimed to disentangle the effects of prenatal and postnatal PCB exposure on neuropsychological development at 4 years of age. This study is based on a population-based birth cohort design established in Menorca (Spain) as part of the INMA [Environment and Childhood] Project. We assessed general neuropsychological development using the McCarthy Scales of Children's Abilities (MCSA). A total of 422 4-year old children were assessed with the MCSA. Levels of PCBs were measured in cord blood (n=405) and in blood samples taken at 4 years (n=285). We found no statistically significant effects of the sum of prenatal PCBs on MCSA scores. Nevertheless, individual congener analyses yielded significant detrimental effects of prenatal PCB153 on the majority of MCSA scores, while no effects were reported for other congeners. The levels of PCBs at 4 years of age were not associated with neuropsychological development. Thus, prenatal exposure to low-level concentrations of PCBs, particularly PCB153, was associated with an overall deleterious effect on neuropsychological development at 4 years of age, including negative effects on executive function, verbal functions and visuospatial abilities, but not on motor development.