Recently, there is ongoing interest in the use of natural plant fibers as alternatives for conventional reinforcements in cementitious composites. The use of natural plant fibers makes engineering work more sustainable, since they are renewable, biodegradable, energy-efficient, and non-toxic raw materials. In this contribution, a comprehensive experimental program was undertaken to determine the influence of pineapple leaf fiber and ramie fiber on the mechanical properties and mass transport of cement-based composites. The compressive strength, tensile strength, modulus of elasticity, modulus of rupture, fracture energy, flexural toughness, coefficient of capillary water absorption, and chloride diffusion were measured. Natural plant fiber-reinforced cement-based composites (NPFRCCs) containing pineapple leaf fiber and ramie fiber, as compared to the plain control, exhibited a slight reduction in compressive strength and a considerable improvement in tensile strength, modulus of elasticity, modulus of rupture, and flexural toughness; the enhancement was remarkable with a higher fiber content. The coefficient of capillary absorption and chloride diffusion of NPFRCCs were significantly larger than the plain control, and the difference was evident with the increase in fiber content. The present study suggests that the specimen with 2% pineapple leaf fiber content can be used in normal environments due to its superior mechanical properties. However, one should be careful when using the material in marine environments.