Background: Health literacy is an important concept associated with participation in preventive health initiatives, such as falls prevention programs. A comprehensive health literacy measurement tool, appropriate for this population, is required. The aim of this study was to evaluate the measurement properties of the Health Literacy Questionnaire (HLQ) in a cohort of older adults who presented to a hospital emergency department (ED) after a fall. Methods: Older adults who presented to an ED after a fall had their health literacy assessed using the HLQ (n = 433). Data were collected as part of a multi-centre randomised controlled trial of a falls prevention program. Measurement properties of the HLQ were assessed using Rasch analysis. Results: All nine scales of the HLQ were unidimensional, with good internal consistency reliability. No item bias was found for most items (43 of 44). A degree of overall misfit to the Rasch model was evident for six of the nine HLQ scales. The majority of misfit indicated content overlap between some items and does not compromise measurement. A measurement gap was identified for this cohort at mid to high HLQ score. Conclusions: The HLQ demonstrated good measurement properties in a cohort of older adults who presented to an ED after a fall. The summation of the HLQ items within each scale, providing unbiased information on nine separate areas of health literacy, is supported. Clinicians, researchers and policy makers may have confidence using the HLQ scale scores to gain information about health literacy in older people presenting to the ED after a fall. Trial registration: This study was registered with the Australian New Zealand Clinical Trials Registry, number ACTRN12614000336684 (27 March 2014).