Background: Multiple sclerosis (MS) is a chronic autoimmune, inflammatory neurological disease of the central nervous system (CNS), increasing in incidence and prevalence across both developed and developing countries. Cognitive difficulties are common in MS sufferers with 70% experiencing difficulties in higher-level brain functioning such as planning, attention, problem solving, and memory. Computerised cognitive training programmes may hold promise as a treatment option for improving cognitive function in people with MS, subject to exploring and addressing potential barriers to usability and acceptability. Methods: This study aimed to test the usability and acceptability of a computerised cognitive training intervention—Strengthening Mental Abilities Through Relational Training (SMART) —for people with MS, through a mostly qualitative prefeasibility design (n= 12). There were two phases of testing: (1) initial usability testing via a think-aloud protocol (n= 6) and (2) alpha-testing to assess experienced acceptability over a four-week period of engagement (n= 6). Data from the two phases were subjected to Framework Analysis, wherein we deductively applied the Health IT Usability Evaluation Model and Theoretical Framework of Acceptability to assess usability and acceptability, respectively. Results: Results show SMART to have satisfactory usability with participants reacting positively to the formatting, visuality, and process of the interface. Minor suggestions were made on how best to adapt SMART for people with MS, but the programme and facilitative support were generally perceived to be acceptable, with participants expressing positive feelings about taking part in the intervention, despite associated burdens. Conclusions: This prefeasibility study provides preliminary evidence of the usability and acceptability of SMART as a computerised cognitive training programme for people with MS. We conclude that we can now move forward with a feasibility trial of SMART, with the intention of proceeding to a definitive trial with cost-effectiveness analysis.