The beneficial effect of dietary n-3 polyunsaturated fatty acids (PUFAs) on developing hypertension has been repeatedly demonstrated. However, related changes in brain membrane composition and its cognitive correlates have remained unclear. Our study aimed at a comprehensive analysis of behavior and cerebral fatty acid concentration in hypertension after long-term PUFA-rich dietary treatment. Hypertensive and normotensive rats were provided a placebo, or one of two PUFA-enriched diets with a reduced (n-6)/(n-3) ratio for 75 weeks. Exploratory behavior and spatial learning capacity were tested. Systolic blood pressure (BP) was repeatedly measured. Finally, brain fatty acid composition was analyzed by gas chromatography. Hypertensive rats exhibited more active exploration but impaired spatial learning compared to normotensives. Both diets reduced BP, increased PUFA and monounsaturated fatty acid (MUFA) concentration, and reduced saturated fatty acid content in brain. The level of cerebral PUFAs and MUFAs was lower in hypertensive than in normotensive rats. Furthermore, BP positively, while spatial learning negatively correlated with cerebral (n-6)/(n-3) PUFA ratio. We concluded that regular n-3 PUFA consumption could prevent the development of hypertension, but reached only a very delicate improvement in spatial learning. Furthermore, we consider a potential role of metabolically generated MUFAs in the beneficial effects of PUFA supplementation.