The growing demand for sustainable alternatives to synthetic composites has increased the interest in natural-fibre-reinforced composites (NFRCs), due to their reduced environmental impact. This study presents a comparative investigation of the mechanical properties of mono-fibre and intraply sisal/flax hybrid composites as cost-effective bio-based solutions. Flax offers high tensile performance but is constrained by higher cost and geographical availability. Sisal, on the other hand, is widely available at lower cost, but exhibits a coarser morphology and reduced processing versatility. Mechanical testing demonstrated that intraply hybrids achieved well-balanced performance, with reduced flax content still delivering competitive tensile strength and stiffness when compared to the higher performing mono-fibre flax composites. However, sisal-rich and hybrid laminates outperformed mono-fibre flax composites in transverse and shear behaviour, with the 67% sisal/33% flax hybrid composite exhibiting the highest transverse properties and the 33% sisal/67% flax hybrid achieving the highest shear properties. Rule-of-mixtures models predicted longitudinal tensile behaviour effectively, while Halpin–Tsai models successfully estimated shear but not transverse and compressive properties. Compressive strength showed limited variation across configurations. Failure analysis identified intra-yarn fracture in flax, limited resin infiltration in sisal, and compressive failure modes such as brooming and microbuckling. Overall, intraply sisal/flax hybrid mats provide a structurally efficient, sustainable, and economically viable alternative to mono-fibre natural composites.