Chronological age (CA) may not accurately reflect the health status of an individual. Rather, biological age (BA) or hypothetical underlying “functional” age has been proposed as a relevant indicator of healthy aging. Observational studies have found that decelerated biological aging or Δage (BA-CA) is associated with a lower risk of disease and mortality. In general, CA is associated with low-grade inflammation, a condition linked to the risk of the incidence of disease and overall cause-specific mortality, and is modulated by diet. To address the hypothesis that diet-related inflammation is associated with Δage, a cross-sectional analysis of data from a sub-cohort from the Moli-sani Study (2005–2010, Italy) was performed. The inflammatory potential of the diet was measured using the Energy-adjusted Dietary Inflammatory Index (E-DIITM) and a novel literature-based dietary inflammation score (DIS). A deep neural network approach based on circulating biomarkers was used to compute BA, and the resulting Δage was fit as the dependent variable. In 4510 participants (men 52.0%), the mean of CA (SD) was 55.6 y (±11.6), BA 54.8 y (±8.6), and Δage −0.77 (±7.7). In a multivariable-adjusted analysis, an increase in E-DIITM and DIS scores led to an increase in Δage (β = 0.22; 95%CI 0.05, 0.38; β = 0.27; 95%CI 0.10, 0.44, respectively). We found interaction for DIS by sex and for E-DIITM by BMI. In conclusion, a pro-inflammatory diet is associated with accelerated biological aging, which likely leads to an increased long-term risk of inflammation-related diseases and mortality.