Polymer composites have been utilized across various industries, especially in transportation, for many years. With a growing emphasis on sustainable production resources, the industry increasingly favours composite materials reinforced with natural fibres or particles. Unlike conventional fibres such as glass, carbon, or aramid, natural fibres typically have low compatibility with polymer matrices, often necessitating pretreatment to enhance bonding. In this study, coir fibres were physically and chemically treated with sodium bicarbonate solutions at varying concentrations (5–15%) and immersion durations (0–5 days). The treated fibres were then mixed into epoxy resin and poured into moulds to produce test specimens for evaluating mechanical properties. The fibre content in the composites ranged from 10 to 20%. Statistical analysis revealed that immersion time significantly affects all mechanical properties tested (tensile modulus, tensile strength, strain, and impact strength). Solution concentration significantly influences tensile modulus and strain, while fibre content significantly affects tensile modulus and strength. The conducted optimization shows that the best mechanical properties are achieved with the minimum tested coir fibre content of 10%. Maximum stiffness and strength can be expected with the longest immersion time of 5 days in the highest solution concentration of 15%. The best strain and impact strength properties, however, are observed at the lowest solution concentration of 5%.