This study aimed to determine the prevalence and investigate the constellations of psychological determinants of the COVID-19 vaccine hesitancy among the Bangladeshi adult population utilizing the health belief model-HBM (perceived susceptibility to and severity of COVID-19, perceived benefits of and barriers to COVID-19 vaccination, and cues to action), the theory of planned behavior-TPB (attitude toward COVID-19 vaccine, subjective norm, perceived behavioral control, and anticipated regret), and the 5C psychological antecedents (confidence, constraints, complacency, calculation, and collective responsibility). We compared the predictability of these theoretical frameworks to see which framework explains the highest variance in COVID-19 vaccine hesitancy. This study adopted a cross-sectional research design. We collected data from a nationally representative sample of 1,497 respondents through both online and face-to-face interviews. We employed multiple linear regression analysis to assess the predictability of each model of COVID-19 vaccine hesitancy. We found a 41.1% prevalence of COVID-19 vaccine hesitancy among our study respondents. After controlling the effects of socio-economic, demographic, and other COVID-19 related covariates, we found that the TPB has the highest predictive power (adjusted R2 = 0.43), followed by the 5C psychological antecedents of vaccination (adjusted R2 = 0.32) and the HBM (adjusted R2 = 0.31) in terms of explaining total variance in the COVID-19 vaccine hesitancy among the adults of Bangladesh. This study provides evidence that theoretical frameworks like the HBM, the TPB, and the 5C psychological antecedents can be used to explore the psychological determinants of vaccine hesitancy, where the TPB has the highest predictability. Our findings can be used to design targeted interventions to reduce vaccine hesitancy and increase vaccine uptake to prevent COVID-19.