There is evidence that food outlet access differs according to level of neighbourhood deprivation but little is known about how individual circumstances affect associations between food outlet access and diet. This study explored the relationship between dietary quality and a measure of overall food environment, representing the balance between healthy and unhealthy food outlet access in individualised activity spaces. Furthermore, this study is the first to assess effect modification of level of educational attainment on this relationship. A total of 839 mothers with young children from Hampshire, United Kingdom (UK) completed a cross-sectional survey including a 20-item food frequency questionnaire to measure diet and questions about demographic characteristics and frequently visited locations including home, children's centre, general practitioner, work, main food shop and physical activity location. Dietary information was used to calculate a standardised dietary quality score for each mother. Individualised activity spaces were produced by creating a 1000m buffer around frequently visited locations using ArcGIS. Cross-sectional observational food outlet data were overlaid onto activity spaces to derive an overall food environment score for each mother. These scores represented the balance between healthy and unhealthy food outlets using weightings to characterise the proportion of healthy or unhealthy foods sold in each outlet type. Food outlet access was dominated by the presence of unhealthy food outlets; only 1% of mothers were exposed to a healthy overall food environment in their daily activities. Level of educational attainment moderated the relationship between overall food environment and diet (mid vs low, p = 0.06; high vs low, p = 0.04). Adjusted stratified linear regression analyses showed poorer food environments were associated with better dietary quality among mothers with degrees (β = -0.02; 95%CI: -0.03, -0.001) and a tendency toward poorer dietary quality among mothers with low educational attainment, however this relationship was not statistically significant (β = 0.01; 95%CI: -0.01, 0.02). This study showed that unhealthy food outlets, like takeaways and convenience stores, dominated mothers' food outlet access, and provides some empirical evidence to support the concept that individual characteristics, particularly educational attainment, are protective against exposure to unhealthy food environments. Improvements to the imbalance of healthy and unhealthy food outlets through planning restrictions could be important to reduce dietary inequalities.