Purpose: Whole grains, generally recognised as healthy choices, are not included in most nutrient profiling systems. We tested modifications to the Nutri-Score algorithm to determine whether including whole grains would provide an improved measure of food, and overall diet quality. Methods: The whole-grain content of food, with a minimum cut-point of 25%, was added to the algorithm, following similar methods used to score other health-promoting components such as fibre. We applied and compared the original and the modified Nutri-Score to food composition and dietary intake data from Australia, France, the United Kingdom, and the United States. Results: At the food level, correlations between whole-grain content and food nutritional score were strengthened using the modified algorithm in Australian data, but less so for the other countries. Improvements were greater in grain-specific food groups. The largest shift in Nutri-Score class was from B to A (best score). At the dietary intake level, whole-diet nutritional scores for individuals were calculated and compared against population-specific diet-quality scores. With modifications, correlations with diet-quality scores were improved slightly, suggesting that the modified score better aligns with national dietary guidelines. An inverse linear relationship between whole-diet nutritional score and whole-grain intake was evident, particularly with modifications (lower whole-diet nutritional score indicative of better diet quality). Conclusion: Including a whole-grain component in the Nutri-Score algorithm is justified to align with dietary guidelines and better reflect whole grain as a contributor to improved dietary quality. Further research is required to test alternative algorithms and potentially other nutrient profiling systems.