Epidemiological evidence suggests an inverse association between whole grain consumption and the risk of non-communicable diseases, such as CVD, type 2 diabetes, obesity and some cancers. A recent analysis of the National Diet and Nutrition Survey rolling programme (NDNS-RP) has shown lower intake of whole grain in the UK. It is important to understand whether the health benefits associated with whole grain intake are present at low levels of consumption. The present study aimed to investigate the association of whole grain intake with intakes of other foods, nutrients and markers of health (anthropometric and blood measures) in the NDNS-RP 2008–11, a representative dietary survey of UK households. A 4-d diet diary was completed by 3073 individuals. Anthropometric measures, blood pressure levels, and blood and urine samples were collected after diary completion. Individual whole grain intake was calculated with consumers categorised into tertiles of intake. Higher intake of whole grain was associated with significantly decreased leucocyte counts. Significantly higher concentrations of C-reactive protein were seen in adults in the lowest tertile of whole grain intake. No associations with the remaining health markers were seen, after adjustments for sex and age. Over 70 % of this population did not consume the minimum recommend intake associated with disease risk reduction, which may explain small variation across health markers. Nutrient intakes in consumers compared with non-consumers were closer to dietary reference values, such as higher intakes of fibre, Mg and Fe, and lower intakes of Na, suggesting that higher intake of whole grain is associated with improved diet quality.