Studies suggest that acute pesticide poisonings (APP) may be linked with long-term neurological effects. To examine long-term neurological and psychological distress symptoms associated with having experienced an APP, we conducted a cross-sectional study of 300 conventional and organic smallholder farmers from Zarcero County, Costa Rica, May–August 2016. We collected self-reported data on sociodemographic characteristics, occupational history, pesticide exposure, APPs, neurological and psychological distress symptoms (using the Brief Symptom Inventory (BSI)). Adjusted logistic regression models were fit. A total of 14% of the farmers (98% male) reported experiencing at least one APP during their lifetime. Self-reported APP was associated with neurological symptoms during the 12 months prior to interview (e.g., fainting (Odds Ratio: 7.48, 95% Confidence Interval: 1.83, 30.74), shaking hands (3.50; 1.60, 7.60), numbness/tingling in hands or feet (3.23; 1.66, 6.32), insomnia (2.53; 1.34, 4.79), accelerated heartrate (2.42; 1.03, 5.47), dizziness (2.38; 1.19, 4.72), increased irritability/anger (2.37; 1.23, 4.55), low energy (2.33; 1.23, 4.46), and difficulty concentrating (2.01; 1.05, 3.85)). Farmers who reported an APP in the ten years prior to interview experienced increased odds of abnormal BSI scores for hostility (4.51; 1.16, 17.70) and paranoid ideation (3.76; 0.99, 18.18). Having experienced an APP may be associated with long-term neurological and psychological distress symptoms.