We described the contribution of ultra-processed foods in the U.K. diet and its association with the overall dietary content of nutrients known to affect the risk of chronic non-communicable diseases (NCDs). Cross-sectional data from the U.K. National Diet and Nutrition Survey (2008–2014) were analysed. Food items collected using a four-day food diary were classified according to the NOVA system. The average energy intake was 1764 kcal/day, with 30.1% of calories coming from unprocessed or minimally processed foods, 4.2% from culinary ingredients, 8.8% from processed foods, and 56.8% from ultra-processed foods. As the ultra-processed food consumption increased, the dietary content of carbohydrates, free sugars, total fats, saturated fats, and sodium increased significantly while the content of protein, fibre, and potassium decreased. Increased ultra-processed food consumption had a remarkable effect on average content of free sugars, which increased from 9.9% to 15.4% of total energy from the first to the last quintile. The prevalence of people exceeding the upper limits recommended for free sugars and sodium increased by 85% and 55%, respectively, from the lowest to the highest ultra-processed food quintile. Decreasing the dietary share of ultra-processed foods may substantially improve the nutritional quality of diets and contribute to the prevention of diet-related NCDs.