Medicines optimisation ensures that people get the best possible outcomes from their medicines. As those with severe mental illness (SMI) are frequently prescribed psychotropic medicines with potentially significant side-effects, poor adherence to treatment and physical morbidity are common. This results in suboptimal symptom control, physical health problems and negative health outcomes. The specialist mental health pharmacist (SMHP) is best placed to provide leadership for medicines optimisation in the inpatient mental health setting. By adopting a patient-centred approach to providing information, improving adherence, screening, initiating and maintaining medicines, and supporting self-advocacy, the SMHP can ensure the patients’ experience of taking medicines is optimised. As there is currently limited understanding of what a baseline clinical pharmacy service in a mental health setting looks like, we aim to outline a framework for pharmacist-led medicines optimisation for those with SMI. This framework is suitable to be scaled and adapted to other settings.