Recent studies confirmed that introducing nanoprecipitates as strengthening phase into high-entropy alloys (HEAs) is an extremely effective means to achieve the excellent strength-ductility synergy. In this work, we successfully created a dual nanoscale precipitate structure in a Co-free Ni2.5CrFeAl0.3Ti0.2 HEA by controlling thermo-mechanical process. Compared to the recrystallized alloy, homogeneous L12 precipitates in FCC matrix and heterogeneous L12/BCC precipitates near grain boundaries were formed in the aged alloys. The dual-nanoprecipitate structure induces a long-range back stress during deformation process, effectively contributing to a balance of high strength and good ductility at 298K. Especially, the mechanical properties of the recrystallized and aged alloys are dramatically improved without strength-ductility tradeoff, showing a multiple-stage strain-hardening behavior at 77 K. In the aged alloys, the nanoprecipitates shorten the mean free path of dislocation movement to effectively induce the precipitation strengthening appreciably depending on the precipitation size. Different from planar dislocations slip dominated by stacking faults at 298K, multiple stacking fault networks and deformation twins were activated sequentially with increasing the tensile strain, thus forming a dynamic Hall-Petch effect at 77K. The current work could help to understand the correlation between mechanical properties and deformation mechanisms in precipitation-strengthening HEAs, and the transformation of these deformation mechanisms provide an insight for developing outstanding-performance HEAs through trigging various hardening modes.