Background: Slow walking speed, time to perform the five-times-sit-to-stand (FTSS) test and motoric cognitive risk syndrome (MCR; defined as slow gait speed combined with subjective cognitive complaint) have been separately used to screen older individuals at risk of cognitive decline. This study seeks to (1) compare the characteristics of older individuals with MCR, as defined through slow walking speed and/or increased FTSS time; and (2) examine the relationship between MCR and its motor components as well as amnestic (a-MCI) and non-amnestic (na-MCI) Mild Cognitive Impairment. Methods: A total of 633, individuals free of dementia, were selected from the cross-sectional “Gait and Alzheimer Interactions Tracking” study. Slow gait speed and increased FTSS time were used as criteria for the definition of MCR. Participants were separated into five groups, according to MCR status: MCR as defined by (1) slow gait speed exclusively (MCRs); (2) increased FTSS time exclusively (MCRf); (3) slow gait speed and increased FTSS time (MCRsaf); (4) MCR; irrespective of the mobility test used (MCRsof); and (5) the absence of MCR. Cognitive status (i.e., a-MCI, na-MCI, cognitively healthy) was also determined. Results: The prevalence of MCRs was higher, when compared to the prevalence of MCRf (12.0% versus 6.2% with P ≤ 0.001). There existed infrequent overlap (2.4%) between individuals exhibiting MCRs and MCRf, and frequent overlap between individuals exhibiting MCRs and na-MCI (up to 50%). a-MCI and na-MCI were negatively [odd ratios (OR) ≤ 0.17 with P ≤ 0.019] and positively (OR ≥ 2.41 with P ≤ 0.019) related to MCRs, respectively. Conclusion: Individuals with MCRf are distinct from those with MCRs. MCRf status does not relate to MCI status in the same way that MCRs does. MCRs is related negatively to a-MCI and positively to na-MCI. These results suggest that FTTS cannot be used to define MCR when the goal is to predict the risk of cognitive decline, such as future dementia.