Background: Nonalcoholic fatty liver disease (NAFLD) is correlated with low-grade inflammation and dietary habits. Until today, there have been limited epidemiologic data assessing the role of diet’s inflammatory potential on NAFLD. The aim was to evaluate the relationship between an anti-inflammatory diet, as reflected by the Dietary Anti-Inflammation Index (D-AII), and NAFLD among cardiovascular disease (CVD)-free adults. Methods: ATTICA is a prospective, population-based study that recruited 3042 adults without pre-existing CVD from the Greek population (Whites; age ⩾18 years; 1514 men and 1528 women). D-AII was calculated using a standard procedure. The baseline study captured various sociodemographic, lifestyle and clinical characteristics as well as hepatic markers. These were used to calculate four NAFLD assessment indices: triglyceride-glucose (TyG) index, fatty liver index (FLI), hepatic steatosis index (HSI), and NAFLD Fatty Liver Score (NAFLD-FLS). Specific cutoffs were applied to capture NAFLD. Results: D-AII showed a significant inverse association with NAFLD, applying the four indices with NAFLD cutoffs [odds ratio (OR) with 95% confidence interval (CI); TyG (0.95, 0.93–0.98); HSI (0.89, 0.86–0.92); FLI (0.88, 0.85–0.91); NAFLD-FLS (0.89, 0.86–0.92)], after adjusting for various confounders. Participants in the highest D-AII tertile had lower odds of having NAFLD, compared with those in the lowest D-AII tertile [(OR, 95% CI); TyG (0.33, 0.24–0.47); HSI (0.13, 0.08–0.23); FLI (0.05, 0.02–0.11); NAFLD-FLS (0.13, 0.07–0.23)]. Anti-inflammatory nutrition was related to lower odds of NAFLD among daily alcohol drinkers and individuals with metabolic syndrome. Conclusions: Anti-inflammatory diet is an important predictor of NAFLD among adults without pre-existing CVD. Adherence to a high anti-inflammatory diet seems to contribute to NAFLD prevention.