With the emergence of the Mobility as a Service (MaaS) concept, it is important to understand whether it has the potential to support behaviour change and the shift away from private vehicle ownership and use. This paper aims to identify potential ways that MaaS (specifically MaaS plans) could help encourage behavioural change; and understand the barriers to using alternative transport modes. In-depth interviews and qualitative analysis are applied to the case study of London. The results indicate that individuals segment the transport modes offered via MaaS into three categories: essential, considered and excluded. Soft measures should target each individuals’ consideration set as this is where the most impact can be made regarding behaviour change. Respondents also highlighted factors that make them apprehensive towards certain modes, such as safety, service characteristics and administration. Interventions that focus on the socio-demographic groups that are most affected could help make these modes more appealing.