Background: Pakistan’s immunization uptake rates are still significantly lower than anticipated despite several initiatives. Lack of awareness, forgetting about vaccination schedule, and vaccine misconception/misinformation are a few of the major drivers that mitigate the rates of immunization. The current COVID-19 pandemic emphasizes the importance of immunization. The significant reductions in regular childhood vaccination during pandemic have increased the risk of outbreaks of vaccine-preventable diseases. Concerns among parents over possibly exposing their children to COVID-19 during child visits may have contributed to the reported declines. Innovative and cost-effective mHealth interventions must be implemented in order to address the problem of inadequate immunization rates. In addition, it is also critical to understand the end user needs in order to reflect on the highly relevant essence of the customized healthcare experience. Objective: The aim of this study was to learn about caregivers’ attitudes toward the usability and acceptability of behavior-change smartphone applications (mobile phones) for improving immunization coverage in Pakistan. Methods: A mixed-method design was employed for this study. The study was conducted at Aga Khan University, Hospital. Parents visiting the Community Health Center for 6-week vaccination of their children were recruited. The study was conducted in two stages. Stage 1 consisted of qualitative interviews that grasped the parent’s attitudes and challenges to immunization, as well as their acceptability and accessibility of the smartphone-based behavior-change application to increase vaccine uptake. Stage 1 was followed by stage 2, in which data were collected through a questionnaire designed by using data from qualitative interviews. Results: The majority of participants agreed that immunization serves an important role in protecting their child from illnesses that cause morbidity and mortality. Almost all of them emphasized the importance of using a pre-appointment method at vaccination center in order to reduce the waiting time. Furthermore, participants were also interested in AI-based behavior modification applications related to immunization. They also wanted to have applications in their native language for better understanding and communication of related information. In our study, approximately 95.2 percent of participants agreed to accept SMS immunization updates, which was also reasonably high. Lastly, the majority of them identified forgetfulness as a significant contributor to regular immunization. Conclusion: To enhance the uptake of childhood vaccines, overall vaccination rates, and overcome barriers related to vaccination coverage, cost-effective and user-friendly mHealth AI-based smart phone applications are required to raise awareness regarding the continuation of vaccination service and the importance of timely vaccination. Parents’ experiences and attitudes must be considered while designing and evaluating the efficacy of mHealth-based interventions.