Age-related deficits in plantar flexor muscle function during the push-off phase of walking likely contribute to the decline in mobility that affects many older adults. Isolated strengthening of the plantar flexor muscles has failed to improve push-off power or walking economy in this population. New mobility aids and/or functional training interventions may help slow or prevent ambulatory decline in the elderly. The overarching objective of this study was to explore the feasibility of using an untethered, dual-mode ankle exoskeleton for treating walking disability in the elderly; testing the device in assistance mode as a mobility aid to reduce energy consumption, and as a resistive gait training tool to facilitate functional recruitment of the plantar flexor muscles. We recruited 6 older adults between the ages of 68 to 83 years to evaluate the feasibility of the dual-mode exoskeleton across two visits. On the first visit, we quantified acute metabolic and neuromuscular adaption to ankle exoskeleton assistance during walking in older adults, and subsequently determined if higher baseline energy cost was related to an individual's potential to benefit from untethered assistance. On the second visit, we validated the potential for push-off phase ankle resistance combined with plantar pressure biofeedback to facilitate functional utilization of the ankle plantar flexors during walking. We also conducted a twelve-session ankle resistance training protocol with one pilot participant to explore the effects of gait training with wearable ankle resistance on mobility and plantar flexor strength. Participants reached the lowest net metabolic power, soleus variance ratio, and soleus iEMG at 6.6 ± 1.6, 19.8 ± 1.6, and 5.8 ± 4.9 minutes, respectively, during the 30-minute exoskeleton assistance adaptation trial. Four of five participants exhibited a reduction (up to 19%) in metabolic power during walking with assistance relative to baseline, but there was no group-level change. Participants who had greater baseline metabolic power exhibited a greater reduction during walking with assistance. Walking with resistance increased stance-phase soleus iEMG by 18 - 186% and stance-phase average positive ankle power by 9 - 88% compared to baseline. Following ankle resistance gait training, the participant exhibited a 5% increase in self-selected walking speed, a 15% increase in fast walking speed, a 36% increase in 6-min-walk-test distance, and a 31% increase in plantar flexor strength compared to pre-intervention measurements. Our results suggest that dual-mode ankle exoskeletons appear highly applicable to treating plantar flexor dysfunction in the elderly, with assistance holding potential as a mobility aid and resistance holding potential as a functional gait training tool. We used an untethered design to maximize the relevance of this for informing the design of intervention studies that may take place at home and in the community to improve mobility and quality of life in older adults. Future studies with larger sample sizes are recommended to expand on the results of this feasibility investigation.