BACKGROUND: Structured Medication Reviews (SMRs) were introduced into primary care in England for patients living with multiple long-term conditions (MLTCs), polypharmacy, increased frailty, in care homes or at risk of medicines-related harm. SMRs aim to optimise the therapeutic potential of medication and reduce medicine-related harms through holistic reviews. AIM: To explore the day-to-day work being undertaken with, and by, clinical pharmacists to implement, embed and integrate SMRs into practice, and consider how to optimise SMRs. DESIGN AND SETTING: Qualitative one-to-one interviews with clinical pharmacists undertaking SMRs and SMR service leaders/managers (SMR leads) in England between February 2023 and November 2024. METHOD: Participants were recruited as part of a wider evaluation of the roll-out of SMRs in England. Interview topic guides and qualitative data analysis were informed by Normalization Process Theory (NPT). RESULTS: Eighteen clinical pharmacists and five SMR leads participated. Participants reported often having to explain the purpose of SMRs and clinical pharmacists' roles to patients, partly due to patients not being informed about SMRs. Participants valued SMRs and expressed that trust-building and tailored consultations were important for optimising medications. Integration varied due to high workload, inconsistent leadership support, inadequate administrative/pharmacist technician resource and lack of training. However, participants described SMRs as valuable for identifying and addressing unmet needs and supporting holistic, person-centred care across MLTC pathways. CONCLUSION: The findings demonstrate the need for improved information on SMRs for patients and primary care teams, adequate and appropriate resource allocation, and enhanced support for consultation skills training to optimise medicines use.