Partridgeberry (Vaccinium vitis-idaea L.) is a good source of food and pharmaceutical ingredients, for which cultivation interest is increasing in North America. Nutrition-oriented breeding programs will benefit from an understanding of how the environment affects the biochemical traits of interest in wild populations. Total phenolic content (TPC) and antioxidant capacity (AC) as measured by the ability to capture free radicals were evaluated simultaneously in leaves and fruit of 56 wild populations across Newfoundland and Labrador, Canada. We tested variation in TPC and AC as a function of eight environmental factors, which showed different effects in leaves and fruit. Contrary to our expectations, TPC was not correlated with AC in either leaves or fruit, and mean TPC and AC were higher in fruit than in leaves. We propose a series of environment-based models for the selection of wild populations. Models for fruit involved ecoregion, temperature, and coastal proximity, and explained up to 51% of variation. While leaf models included surface water pH and sensitivity to acid rain, explaining up to 31%. We conclude that wild population selection in the province should target the North Shore Forest ecoregion and warm temperatures for fruit; and regions with low water alkalinity and pH > 6.6 for leaves.