To effectively address medication adherence and improve cardiovascular health among older adults, a deeper understanding is needed of the barriers that this age group faces and of approaches that would be most effective and feasible for improving adherence. We conducted a focus group study (n = 25) in a diverse population of older adults with hypertension recruited from the Cohort Study of Medication Adherence in Older Adults (CoSMO). A structured guide was used to collect feedback on barriers to adherence and acceptability and the feasibility of intervention strategies. The final coding framework outlines factors at the individual, relationship, health care system, and environmental or policy level that affect adherence in older adults. These include memory, knowledge, attitudes and beliefs, side effects, social support, interaction with healthcare providers, and cost and convenience of medication filling. Patient responses highlighted the varied nature of barriers and the need for interventions that are both multifaceted and tailored.