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Background Environmental exposure to pesticides has been linked to adverse mental and cognitive outcomes. Rural zones in Chile’s Maule Region face chronic exposure to agrochemicals due to overlapping agricultural, forestry, and industrial activities.Objective To examine associations between pesticide residues in environmental matrices and adult mental health and neurocognitive indicators in rural communities.Methods This cross-sectional study included 95 adults residing within 10 km of agricultural and agro-industrial sources in San Javier and Cauquenes. Soil, water, and fly samples were analyzed via GC-MS/MS for organophosphates and pyrethroids. Mental health and cognitive functioning were assessed using CES-D, STAI, GHQ-12, SF-12, MMSE, and IFS. Robust multivariate regressions (Huber-IRLS) and Spearman correlations were used to assess associations, adjusting for confounders.Results Chlorpyrifos in water exceeded WHO limits (max: 61.6 µg/L vs. 30 µg/L); diazinon reached 4.58 µg/L (WHO limit: 0.1 µg/L). Multivariate models showed that cypermethrin in water was significantly associated with higher depressive symptoms (CES-D; β = 0.90, p = 0.008), and chlorpyrifos in water was inversely associated with quality of life (SF-12; β = –0.21, p = 0.002). Cypermethrin in soil was linked to poorer executive function (IFS; β = –4.94, p = 0.003). Spearman correlations confirmed spatial associations: chlorpyrifos levels were higher near vineyards (ρ = –0.43), and cypermethrin near forestry zones (ρ = –0.35). A high proportion of participants reported strong odor nuisance (85%) and rated it unacceptable (90%).Conclusions Simultaneous environmental exposure to organophosphate and pyrethroid pesticides is significantly associated with mental health deterioration and cognitive impairment in rural populations. These findings call for integrated environmental and public health interventions, especially in underserved agricultural regions.