Acrylamide exposure, mainly resulting from food cooking and processing, has been associated with a higher risk of health problems, due to genotoxic effects. This study aims to estimate acrylamide dietary exposure of the Portuguese population and its associated factors. Dietary data collected through 2 non-consecutive 24 hour recalls or food diaries from a representative sample of the Portuguese population from the National Food, Nutrition and Physical Activity Survey was used (n = 5811; 3–84 years). Occurrence data of acrylamide in food were obtained from EFSA. The margins of exposure (MOE) were calculated for peripheral neuropathy and neoplastic effects. The association between acrylamide and socio-demographic characteristics was estimated through linear regression models. For the total population, the estimated median daily dietary exposure per body weight to acrylamide was 0.38 µg/kg/day, ranging from 0.14 to 0.88 µg/kg/day for the 5th and 95th percentile, respectively. Children aged between 1–2 years had the highest acrylamide exposure (median 0.75 µg/kg/day, 95th percentile 1.41 µg/kg/day). For the peripheral neuropathy and neoplastic effects, the median MOE estimated was 1140 and 451, respectively. Men compared to women had a higher acrylamide dietary exposure, as well as smokers compared to non-smokers. Elderly and less educated individuals were inversely associated with acrylamide exposure. ‘Bread and rusks’ (24.2%) were the main source of acrylamide, followed by ‘coffee’ (21.3%). The current dietary exposure to acrylamide in the Portuguese population is of concern mainly regarding neoplastic effects. Our results point to the need to reduce exposure to acrylamide, especially in men, young children, higher educated individuals and smokers.