The emergence of SARS-CoV-2 mutants, waning immunity, and breakthrough infections prompted the use of booster doses of the COVID-19 vaccine to fight against the pandemic. India started booster doses in January 2022 and it is critical to determine the intention of booster dose uptake and its correlates. Therefore, the current cross-sectional study aimed to investigate booster dose acceptability and associated predictors among the Indian population. A convenience sampling technique was utilized to recruit a sample of 687 Indian residents. A 55-item psychometric validated survey tool was used to assess booster dose acceptability, vaccine literacy and vaccine confidence. Univariate, bivariate, and multivariate statistical methods were used to analyze the data. Over 50% of participants reported their willingness to take the booster dose. Among the group not willing to take the booster dose (n = 303, 44.1%), a significantly larger proportion of respondents were unvaccinated with the primary series (12.2% vs. 5.2%, p < 0.001), had an annual income below 2.96 lacs/annum (52.8% vs. 33.1, p < 0.001), were residents of rural areas (38.0% vs. 23.2%, p < 0.001), were not living with vulnerable individuals (78.5% vs. 65.2%, p < 0.001) and did not have family/friends who had tested positive for COVID-19 (54.6% vs. 35.1%, p = 0.001). Demographic, vaccine variables and multi-theory model subscales to predict the initiation of booster dose among hesitant participants were statistically significant, R2 = 0.561, F (26, 244) = 11.978, p < 0.001; adjusted R2 = 0.514. Findings of this study highlight the need to develop evidence-based interventions to promote vaccine uptake, particularly among hard-to-reach communities living in developing countries.