<p>The association between physical function and working memory in older adults is moderated by structural dimensions of physical function, but it is unclear which structural dimensions of physical function are associated with working memory in healthy older adults. The purpose of this study was to construct the structural dimensions of physical function and assess their associations with working memory in adults aged 60–74 years to provide potential targets for earlier identification and interventions of physical function and working memory decline in older adults. To this end, data from 664 to 589 eligible older adults were used for factor analysis and structural equation modeling, respectively. A constructed structural model of three factors of physical function had good reliability and validity. The structural dimensions of physical function in adults aged 60–74 years were mobility and dynamic balance, muscular strength and cardiorespiratory endurance. Physical function in older adults was closely associated with working memory, with mobility and dynamic balance—but not muscular strength and cardiorespiratory endurance— closely associated with working memory.</p>