While rates of mild cognitive impairment (MCI) are relatively high in populations with cardiovascular diseases and risk factors, screening tests for MCI have not been evaluated in this patient group. This study investigated the sensitivity and specificity of the Montreal Cognitive Assessment (MoCA) tool for detecting MCI in 110 patients (mean age 67.9 + 11.7 years; 60% female) recruited from hospital cardiovascular outpatient clinics. Mean MoCA performance was relatively low (22.8 + 3.8) in this group, with 72.1% of participants scoring below the recommended cutoff for cognitive impairment (<26). The presence of MCI was determined using the Neuropsychological Assessment Battery Screening Module (NAB-SM). Both amnestic MCI and multiple-domain MCI were identified. The optimum MoCA cutoff for detecting MCI in this group was <24. At this cutoff, the MoCA's sensitivity for detecting amnestic MCI was 100% and for multiple-domain MCI it was 83.3%. Specificity rates for amnestic MCI and multiple-domain MCI were 50.0% and 52% respectively. The poor specificity of the MoCA suggests that it will have limited value as a screening test for MCI in settings where the overall prevalence of MCI is low.