Objective Test the feasibility of assessing cognition, psychiatric symptoms and daily living skills of potential brain donors by telephone and compare satisfaction and attitudes across telephone and face‐to‐face assessment. Method Data were collected from 108 healthy participants from the Brains for Dementia Research cohort. Purposive sampling was used to assess feasibility and a randomised control trial design compared satisfaction and attitudes towards telephone and face‐to‐face assessment. Non‐parametric tests were conducted to compare groups, and logistic regression was performed to assess the relationship between satisfaction and participant characteristics. Results Of the 80 participants offered telephone assessment, 67 (83.8%) agreed, 2 (2.5%) had a significant hearing impairment, 4 (5.0%) had potential memory problems and 7 (8.7%) declined. On average, telephone assessments lasted 38 min and duration was negatively associated with Telephone Interview of Cognitive Status‐Modified scores (p = 0.001) and positively associated with age (p = 0.040), Neuropsychiatric Inventory scores (p = 0.019), Geriatric Depression Scale (p = 0.035) and Global Deterioration Scale (p = 0.022). Satisfaction was high in respect to organisational and personal aspects; ratings did not differ significantly across telephone and face‐to‐face assessment groups and were not related to socio‐demographic characteristics. Participants undergoing telephone assessment were significantly more likely to hold positive attitudes towards this mode of assessment. Conclusions Telephone assessment is feasible, time‐efficient and acceptable to healthy, potential brain donors. When used with other assessment modes and within the context of established contact, telephone assessment offers greater flexibility to researchers and participants and represents an effective mechanism for overcoming the challenges of growing, ageing cohorts and uncertain resources. Copyright © 2016 John Wiley & Sons, Ltd.