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BACKGROUND Exclusive breastfeeding (EBF) through 6 months of age in most low- and middle-income countries (LMICs) is surprisingly low. In India, an LMIC, EBF rates fall well below the World Health Organization benchmark of 90%. There has been a relative lack of mobile health (mHealth) applications that specifically focus on leveraging the use of peer counselors (PCs) to support mothers as a means of increasing exclusive breastfeeding practices in LMICs. OBJECTIVE A key study objective was to design, develop, and test the usability of BEST4Baby, a mHealth app specifically designed to support PCs in providing in-home breastfeeding counseling support to mothers in rural India around optimal breastfeeding practices. METHODS To develop and test BEST4Baby, we applied behavioral theories (i.e., social cognitive theory and theory of planned behavior) to a user-centered design (UCD) process with an Agile development methodology. The approach involved stakeholders and PCs to guide BEST4Baby’s design and development including the app’s content and features. PCs were engaged through the use of focus groups with interactive wireframes. Their feedback helped finalize the design prior to development. During the 24-month study period, we conducted a feasibility test of the BEST4Baby app with 23 PCs that supported mothers residing in rural India in a pilot study that incorporated an intervention (n=110) and control (n=112) group. The intervention protocol required PCs to provide education and follow mothers using BEST4Baby from the late prenatal stage of pregnancy through 6 months postpartum. BEST4Baby’s usability from the PCs’ perspective was assessed using a translated System Usability Scale (SUS). RESULTS The findings of this study align with best practices in UCD (i.e., understand user experience, context with iterative design with stakeholders) to address EBF barriers. It led to the cultural tailoring and contextual alignment of an evidence-based WHO breastfeeding program with iterative design and Agile development of the BEST4Baby app. The approach translated to a highly usable BEST4BABY app for employment by PCs for breastfeeding counseling that has been shown to statistically increase EBF practices. PCs rated BEST4Baby as highly usable, scoring it over the 95th percentile on the SUS scale. CONCLUSIONS Findings suggest that BEST4Baby was highly usable and accepted by PCs in supporting mothers in their EBF practices and led to positive outcomes in the intervention group’s EBF rates. The pilot demonstrated that the use of the specially designed BEST4Baby app was an important support tool for PCs during the nine home visitations.