To collect data for fusion applications and understand the basic properties of tungsten, single-crystal tungsten was neutron irradiated in the mixed-spectrum High Flux Isotope Reactor at the Oak Ridge National Laboratory at temperatures of 90–830 °C to fast fluences of 0.01–9 × 1025 n/m2 (E > 0.1 MeV). For tensile tests at room temperature of the irradiated material in both orientations, <110> and <100> tensile orientation, initially there was strengthening that peaked at 0.02 dpa and was followed by progressive modulus of toughness reduction, approaching zero at higher doses. For all irradiation temperatures, in elevated temperature tensile tests there was a distinct transition from ductile-to-brittle behavior between 0.1 and 0.4 dpa, accompanied by an increase in indentation hardness. The ductile-to-brittle transition with increasing dose was particularly critical because it presented as a total loss in elongation and modulus of toughness. The critical transition dose was well below the dose (∼1 dpa) where irradiation-induced precipitates are visible in the TEM. The extent of Vickers microhardness increase was significant at higher doses and did not depend on irradiation temperature or crystal orientation, reaching 12.9 GPa after 2.8 dpa. The significant mechanical property degradation above 0.1 dpa is believed to have been caused by the accumulation of irradiation-induced clusters and eventually precipitates of the transmutation elements Re and Os.