<p>To overcome the limitation of insufficient room-temperature strength in face-centered cubic (FCC) single-phase high-entropy alloys (HEAs), CrFeCoNiAl_xTi_2−x powders and bulk specimens were fabricated via mechanical alloying (MA) combined with spark plasma sintering (SPS). The regulatory effects of ball milling parameters and Al/Ti molar ratio on the microstructure evolution and mechanical properties of the alloys were systematically explored. Results demonstrated that the optimal ball milling duration for mechanical alloying was 10&#xa0;h and the powders achieved atomic-scale interdiffusion forming stable FCC + BCC dual-phase solid solution with uniform particle distribution and no obvious elemental segregation. The Al/Ti molar ratio regulated the dynamic equilibrium between cold welding and fracturing as well as the atomic diffusion efficiency influencing the powder morphology, bulk microstructure and phase composition. With the decreasing Al content and the increasing Ti content, the bulk alloys exhibited increasing precipitation of hard Laves phases and the grains evolving from fine equiaxed grains to coarse blocky grains. Mechanical property realized lightweight design with relative densities higher than 93%. The microhardness increased with the increasing of Ti content and the CrFeCoNiAl_1.5Ti_0.5 alloy exhibited the highest hardness. The CrFeCoNiAl₁Ti₁ alloy achieved the optimal strength-ductility synergy with compressive strength of 1952.89&#xa0;MPa and plastic strain of 4.01% accompanying by low-strain rate sensitivity. TheCrFeCoNiAl_0.5Ti_1.5 alloy possessed the lowest friction coefficient and excellent wear resistance, which was attributed to form a dense and continuous <i>α</i>-Al₂O₃ oxide film during friction. This paper provided experimental data and theoretical guidance for the alloy design, process optimization, and engineering applications of high-entropy alloys.</p>