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Introduction Early initiation of antiretroviral therapy (ART) and adequate adherence are associated with sustained viral load (VL) suppression and effective treatment in people living with HIV (PLHIV). Enhanced adherence counseling (EAC) has been recommended for PLHIV on therapy with a VL >1000 copies/mL. We developed a digital application, "Samvaad," for counselors at ART centers to document the barriers to poor adherence and to provide thematic EAC for registered PLHIV under the aegis of the Mumbai District AIDS Control Society. The objectives of this study are to document the barriers to ART adherence in PLHIV who require EAC and to report the suppression outcomes in those who received EAC using Samvaad. Methods This study is a pre-post analysis of retrospective programmatic data from 674 PLHIV across 16 ART centers in Mumbai, India, from September 2020 to July 2022. We included only PLHIV who had unsuppressed VL and/or ART adherence <95% for the present analysis. The main outcome was the change in VL status, from unsuppressed at baseline to suppressed at follow-up assessment. We collected demographic information, ART-related information (duration of ART and type of ART regimen), and CD4 counts at the time of EAC. We also documented barriers to ART adherence using "Samvaad." Results The mean (SD) age of PLHIV was 37.1 (9.9) years; 60.7% (n=409) were male, and 39.3% (n=265) were female. The most common barrier at baseline was "I have not been adequately informed about the dose and schedule of medications" (65.1% (n=439)), followed by "I do not have a fixed time to take my medicines" (63.2% (n=426)). The least common barriers were "I skip medications in the morning whenever I have alcohol the previous night" (4.2% (n=28)), "I skip medications whenever I have a fight with my partner/lover" (4.5% (n=30)), and "I live with a lot of people and hence I am unable to keep the ART medications at home" (4.5% (n=30)). The most common domains were "pill-taking practices" (68.3% (n=460)) and "ART knowledge/behavior" (67.7% (n=456)). At follow-up assessment, about 90% of PLHIV had suppressed VLs. In the multivariate analysis, males were significantly more likely to be virally suppressed compared with females (OR: 1.99, 95% CI: 1.07-3.68; p=0.029). PLHIV on third-line ART (OR: 0.30, 95% CI: 0.11-0.85; p=0.024) and those with the practices barrier domain (OR: 0.44, 95% CI: 0.22-0.90; p=0.024) were significantly less likely to achieve VL suppression at follow-up. Conclusions The majority of PLHIV in our study were between 26 and 45 years of age, were male, had been on ART for more than five years, and were on first-line ART. The main barriers were a lack of adequate knowledge about dosage and side effects, as well as not having a fixed schedule for taking pills. Viral suppression was reported in approximately 90% of PLHIV after EAC sessions. However, VL suppression was less likely in those who did not have a fixed time for taking medicines. This is a practical problem that needs to be addressed by developing treatment plans that consider time spent away from home or in transit. The development of a digital app was useful to document key barriers and domains in PLHIV with poor adherence and to provide thematic EAC at ART centers. The app can be used in urban as well as rural ART centers to provide client-centric thematic adherence counseling.