In recent years, sustainable composites have gained increased attention due to various reasons, such as the depletion of non‐renewable resources, environmental sustainability, and the introduction of plastic pollution. The present work aims to develop biocomposites (with a maximum biological content of 61.78%) based on Bambusa tulda fiber and cashew‐nut shell oil‐based bio‐epoxy resin. Different concentrations of NaOH (2%, 4%, 6%, 8%, and 10%) are used to determine the most suitable NaOH concentration for bamboo fiber treatment. The effect of different treatment concentrations on bamboo fiber has been analyzed by performing single‐fiber tensile testing, fiber pull‐out testing, X‐ray diffraction (XRD), Fourier transform infrared spectroscopy, thermogravimetric analysis, and atomic force microscopy. The investigation revealed that the 6% NaOH‐treated fiber showed better thermo‐mechanical and interfacial properties. Various fiber weight fractions (10%, 20%, 30%, and 40%) are used for composite fabrication, and 30% fiber‐loaded composites show the best mechanical properties. The effect of chemical treatments on the mechanical properties of biocomposites was investigated using composites with a 30% fiber weight fraction and different NaOH treatments. It has been reported that 30% fiber weight fraction 6% NaOH treated composites show better tensile strength (132.916 MPa), tensile modulus (6.983 GPa), flexural strength (154.8 MPa), modulus (8.243 GPa), and impact strength (44.06 kJ/m2) with less moist absorption. The developed composites have shown excellent potential for advanced engineering applications when compared with previously reported composites.