The issue of brittleness and low post-peak load energy associated with the plain HSC led to the development of fiber-reinforced concrete (FRC) by using discrete fiber filaments in the plain matrix. Due to the high environmental impact of industrial fibers and plasticizers, FRC development is ecologically challenged. Sustainability issues demand the application of eco-friendly development of FRC. This study is aimed at the evaluation of coir as a fiber-reinforcement material in HSC, with the incorporation of silica fume as a partial replacement of cement. For this purpose, a total of 12 concrete mixes were produced by using three different doses of coir (0%, 1%, 1.5%, and 2% by wt. of binder) with silica fume (0%, 5%, and 10% as volumetric replacements of cement). The examined parameters include compressive strength, shear strength, splitting tensile strength, ultrasonic pulse velocity, water absorption, and chloride ion permeability. The scanning electron microscopy (SEM) technique was adopted to observe the microstructure of the CF-reinforced concrete. The results revealed that due to the CF addition, the compressive strength of HSC reduces notably; however, the splitting tensile strength and shear strength experienced notable improvements. At the combined incorporation of 1.5% CF with 5% silica fume, the splitting tensile strength and shear strength of the concrete experienced improvements of 47% and 70%, respectively, compared to that of the control mix. The CF incorporation is detrimental to the imperviousness of concrete. The combined incorporation of CF and silica fume is recommended to minimize the negative effects of CF on the permeability resistance of concrete. The SEM results revealed that CF underwent a minor shrinkage with the age.