The world’s population is ageing, with the number of those over 60 years expected to represent a fifth of the total population by 2050. Increases in chronic long-term health conditions (LTCs) associated with ageing, and requiring regular but often avoidable medical intervention, are pressurising already overloaded, health and social care systems. Atrial fibrillation (AF) is an LTC, which is most frequently diagnosed in the elderly. An often, asymptomatic condition, AF is associated with a 3- to 5-fold increased risk of severe ischemic stroke. Stroke prevention, with risk-stratified oral anticoagulants (OACs) is the standard recommended care for patients with AF. Stroke avoidance is, however, dependent on persistent adherence to OAC medication, with an adherence rate of >80% considered necessary to achieve optimal health outcomes. Suboptimal adherence to OACs is common, with a third of all AF patients not taking their medication as prescribed. This combined with the short half-life of OACs can result in poor clinical outcomes for patients. Policy makers now consider improving adherence to prescribed medicines for LTCs, a public health priority, to ensure better health outcomes for patients, whilst minimising unnecessary health system costs. Prescribing medicines to treat LTCs, such as AF, is not enough, particularly when the patient may not experience any measurable benefit to the treatment and may instead, experience medication-associated adverse events, including a risk of bleeding. Pharmacists who are experts in medicines management are ideally placed to support medication adherence, to educate, and to improve health outcomes for patients with AF. In this review, I will consider the evidence for poor medication adherence in LTCs and in particular adherence to OACs in patients with AF and highlight the role that pharmacists can play in ensuring optimal adherence and showcase pharmacist-led interventions that effectively address this problem.