Graphite ore and graphite tailings were blended into iron-tailings-based cementitious mortars, and their mechanical properties and microstructure were experimentally investigated. The flexural and compressive strengths of the resulting material were tested to compare the effects of graphite ore and graphite tailings as supplementary cementitious materials and fine aggregates on the mechanical properties of iron-tailings-based cementitious mortars. Additionally, their microstructure and hydration products were mainly analyzed using scanning electronic microscope and X-ray powder diffraction techniques. The experimental results showed that the mechanical properties of the mortar material incorporating graphite ore were reduced due to the lubricating properties of graphite ore. As a result, the unhydrated particles and aggregates were not tightly bound to the gel phase, making the direct application of graphite ore in construction materials unfeasible. In the iron-tailings-based cementitious mortars prepared in this work, the optimal incorporation rate of graphite ore as a supplementary cementitious material was 4 wt%. The compressive strength of the optimal mortar test block after 28 days of hydration was 23.21 MPa, and the flexural strength was 7.76 MPa. The mechanical properties of the mortar block were found to be optimal with a graphite-tailings content of 40 wt% and an iron-tailings content of 10 wt%, resulting in a 28-day compressive strength of 48.8 MPa and a flexural strength of 11.7 MPa. By observing the microstructure and XRD pattern of the 28-day hydrated mortar block, it was determined that the hydration products of the mortar with graphite tailings as an aggregate included ettringite, Ca(OH)2, and C-A-S-H gel.