Purpose: This study aims to investigate the determinants of individuals’ attitudes toward using Bitcoin and their behavioral intention to use it in Bangladesh. Additionally, it explores the relationship between sustainability and the behavioral intention to use Bitcoin. Design/Methodology/Approach: Utilizing the Technology Acceptance Model (TAM) and Extended Technology Acceptance Model (ETAM), this research develops measurement scales based on prior literature synthesis. Data are collected through a structured web survey distributed across Bangladesh’s eight divisions. Structural Equation Modeling (SEM) is employed to validate the measurement model and analyze the structural relationships between variables. Findings: The findings reveal significant correlations between attitude toward using Bitcoin and behavioral intention to use it, as well as with the sustainability of Bitcoin usage. Usability attributes demonstrate a strong correlation with attitude toward using, while perceived usefulness is found to be influential, highlighting the importance of perceived benefits in shaping user attitudes. Surprisingly, knowledge, perceived ease of use, and security concerns do not significantly affect attitude toward using, suggesting that other factors may outweigh security considerations. Moreover, sustainability significantly influences the behavioral intention of Bitcoin adoption. Originality: This study provides valuable insights for policymakers, businesses, and researchers aiming to promote the sustainable adoption of Bitcoin and other cryptocurrencies. It underscores the significance of perceived benefits and usability features in shaping user attitudes and intentions in emerging markets like Bangladesh.