Theobromine, a bioactive compound found in cacao beans, is recognized for its pharmacological health benefits, such as improving heart health by lowering blood pressure, enhancing cognitive function, supporting respiratory health, providing antioxidant benefits, reducing inflammation, and promoting dental health. However, its limited solubility in water poses challenges for therapeutic applications, necessitating methods to enhance its solubility. The approach to enhance its bioavailability making it more effective for medicinal use and easier to incorporate into various pharmaceutical and nutraceutical products. Hydrotropic solubilization, utilizing the amphiphilic nature of sodium benzoate, is employed to improve the solubility of theobromine. Through systematic investigation of varying concentrations (0–3 mol/L) of sodium benzoate and temperature conditions ranging between 303 and 333 K, this study is aimed to elucidate their effects on the solubility of theobromine. Standardized protocols were utilized to measure the concentration of dissolved theobromine in sodium benzoate solutions, while thermodynamic properties were analyzed to understand the underlying mechanism. The study discovered that the solubility of theobromine was enhanced by sevenfold in the presence of sodium benzoate. Thermodynamic analysis revealed the solubilization process to be entropy-driven. Additionally, contact angle estimations confirmed increased hydrophobicity with higher sodium benzoate concentration, facilitating the solubilization of theobromine in the aqueous phase. Furthermore, FTIR analysis indicates that the solubilization of the bioactive compound occurs exclusively subsequent to traversing the minimum hydrotropic concentration (MHC).