Background: Older adults living in long-term care (LTC) are nutritionally vulnerable. The purpose of this study was to determine diet quality of Canadian LTC residents and its association with malnutrition and low calf circumference. Methods: A cross-sectional study was undertaken in 32 LTC homes across four Canadian provinces. Nutrient adequacy ratios (NARs) were calculated for seventeen nutrients; mean adequacy ratio (MAR) was calculated to describe overall diet quality. Malnutrition risk was assessed with the Mini Nutritional Assessment-Short Form (MNA-SF) and diagnosis of protein/energy malnutrition with the Patient-Generated Subjective Global Assessment (PG-SGA). Calf circumference (CC) was also assessed. Linear and logistic regressions for these outcomes with diet quality as the predictor were conducted adjusting for covariates. Results: Average MNA-SF score was 10.7 ± 2.5. Residents (43.5%) had mild/moderate to severe malnutrition based on the PG-SGA and 32.6% had a CC of < 31 cm. Mean MAR score was 0.79 ± 0.09 with significant differences between those requiring eating assistance (0.77 ± 0.11) and those that did not require assistance (0.80 ± 0.07) (p < .05). MAR score was significantly associated with malnutrition in fully adjusted models: MNA-SF scores [β = 5.34, 95% Confidence interval (CI) (2.81, 7.85)] and PG-SGA [Odds ratio (OR) = 0.49, 95% CI (0.38, 0.64)]. Those who had better diet quality were more likely to be well nourished or not at risk. Although several individual nutrients were associated with low CC (< 31 cm), there was no association between overall diet quality (MAR) and low CC. Conclusions: Diet quality is associated with malnutrition and individual nutrients (NARs) with a low CC. In addition to calories and protein, nutrient dense diets that promote adequate micronutrient intake are required in LTC.