Greater use of locally available supplementary cementitious materials (SCM) to reduce cement content and addition of fiber reinforcement can enhance the performance of 3D printing (3DP) technology in construction. In this study, three classes of eco-friendly 3D printable fiber-reinforced mixtures were targeted, namely ultra-high-performance concrete (UHPC), high-performance concrete (HPC), and conventional concrete (CC). A step-by-step methodology was proposed to maximize the substitution rate of cement with SCM and limestone filler and optimize fiber volume for the successful development of 3D printable fiber-reinforced materials. Binder combinations were initially investigated on the paste level to determine the packing density and robustness. Selected binder systems were narrowed down on the mortar level by evaluating the superplasticizer (SP) demand, plastic viscosity, forced bleeding, final setting time, and 3-day compressive strength. The 6-mm steel and 8-mm polyvinyl alcohol (PVA) fibers were incorporated for further evaluation of key properties of fiber-reinforced concrete. The printability of the fiber-reinforced mixtures was validated using an extrusion-based 3D printer. Developing such print materials with adequate strength and toughness can improve the cost-effectiveness of 3DP construction, and extend 3DP technology to remote areas.