Background: The use of mobile health (mHealth) has gained popularity globally, including for its use in a variety of health interventions, particularly through short message service (SMS) text messaging. However, there are challenges to the use of mHealth, particularly among older users who have a large heterogeneity in usability and accessibility barriers when using technology. Objective: In order to better understand and conceptualize the diversity of users and give insight into their particular needs, we turned to persona creation. Personas are user archetypes created through data generated from multi-method inquiry with actual target users. Personas are an appropriate yet largely underutilized component of current mHealth research. Methods: Leveraging data from a multi-method study conducted in Singapore with an ethnically diverse population including Chinese, Malay, and Indian participants, we used a proforma to analyze data from the qualitative component (ie, 20 in-depth interviews) and quantitative component (ie, 100 interviewer-guided surveys). We then identified key characteristics, including technology use and preferences as well as adherence factors, to synthesize five personas reflective of persons over the age of 40 years in Singapore with atherosclerotic cardiovascular disease (ASCVD) or ASCVD risk factors, such as hypertension. Results: We present five personas typologized as (1) The Quiet Analog, (2) The Busy Grandparent, (3) The Socializer, (4) The Newly Diagnosed, and (5) The Hard-to-Reach. We report on four key characteristics: health care access, medication adherence, mobile phone technology usage (ie, ownership, access, and utilization), and interest in mHealth. Finally, we provide insights into how these personas may be used in the design and implementation of an mHealth intervention. Our work demonstrates how multi-method data can create biopsychosocial personas that can be used to explore and address the diversity in behaviors, preferences, and needs in user groups. Conclusions: With wider adoption of mHealth, it is important that we consider user-centered design techniques and design thinking in order to create meaningful, patient-centered interventions for adherence to medications. Future research in this area should include greater exploration of how these five personas can be used to better understand how and when is best to deliver mHealth interventions in Singapore and beyond.