The aim of this study was to determine whether physical and psychological functioning can predict 6-year cognitive decline in older adults. A group of 669 participants aged 60 to 81 years was recruited from a longitudinal study (the Maastricht Aging Study). Physical functioning was measured in terms of perceived health and instrumental activities of daily living. Psychological functioning or mood was evaluated by the Depression and Anxiety subscales of the Symptom Check List-90. Although physical functioning and psychological functioning were related to several measures of cognitive functioning at baseline, psychological functioning was specifically related to memory functioning 6 years later. Poor psychological functioning (i.e., depressive and anxiety symptomatology), rather than poor physical health, may have the strongest implications for long-term cognitive functioning in older men and women.