The effects of various heat treatments on the microstructure and hardness of new Ni56Ti41Hf3 and Ni56Ti36Hf8 (atomic %) alloys were studied to evaluate the suitability of these materials for tribological applications. A solid-solution strengthening effect due to Hf atoms was observed for the solution annealed (SA) Ni56Ti36Hf8 alloy (716 HV), resulting in a comparable hardness to the Ni56Ti41Hf3 alloy containing 54 vol.% of Ni4Ti3 precipitates (707 HV). In the Ni56Ti41Hf3 alloy, the maximum hardness (752 HV), achieved after aging at 300°C for 12 h, was attributed to dense, semi-coherent precipitation of the Ni4Ti3 phase. Unlike the lenticular morphology usually observed within binary NiTi alloys, a "blocky" Ni4Ti3 morphology formed within Ni56Ti36Hf3 due to a smaller lattice mismatch in the direction normal to the habit plane at the precipitate/matrix interface. The maximum hardness for Ni56Ti36Hf8 (769 HV) was obtained after applying an intermediate aging step (300°C for 12 h) followed by normal aging (550 °C for 4 h). This two-step aging treatment induces dense nanoscale precipitation of two interspersed