The aim of this study was to determine the relative validity of the HEalthy LIfe in an Urban Setting (HELIUS) food frequency questionnaire (FFQ) in assessing the dietary intake of energy, nutrients, and food groups of Dutch older men and women. In 2014–2015, 88 participants of the Longitudinal Aging Study Amsterdam aged 71.9 (SD 8.6) years completed the 238-item HELIUS FFQ and three 24-hour dietary recalls. The mean group-level bias in the intakes of energy, nutrients, and food groups between the two methods was assessed, as well as Pearson’s correlation coefficients and level of agreement using quintile distribution. For the intakes of energy and macronutrients, the group-level bias was ≤5%, Pearson’s correlation coefficients were moderate to good (ranging from 0.26 for total fat to 0.72 for alcohol), and agreement was moderate to high (classification in same or adjacent quintile ranging from 63% for energy, protein, and carbohydrate to 91% for alcohol). For most micronutrients and food groups, the relative validity was moderate (Pearson’s correlation coefficients between 0.3 and 0.5), with the lowest correlations for β-carotene (0.08), vitamin B1 (0.19), fish (0.14), and grains (0.24). In conclusion, for energy and macronutrients, most micronutrients, and most food groups, the relative validity of the HELIUS FFQ to assess dietary intake in Dutch older adults was acceptable to good.