In this work, we studied the effect of liquid-phase redox cycling on the size of Cu nanoparticles and oxides. The mixed solution of sodium hydroxide and ammonium persulfate was applied as the oxidation system at room temperature, and ascorbic acid was used as reduction agent at 80 °C in the cycling process. It was found that pristine copper particles with average size of around 800 nm and wide distribution from 300 to 1300 nm could be turned into the resulting particles with the average size of around 162.3 nm with the distribution from 75 to 250 nm after 5 redox cycles. It was also observed that uniform copper oxide nanowires formed after 5 oxidation cycles could be easily reduced into fine copper nanoparticles. The critical tuning factors including the precursor size, morphology, defects, reaction time, and the way of adding oxidant were investigated. It was suggested that the synergetic driving effect of chemical reduction and nanostructure thermodynamic instability in solution accounted for the size reformation of the copper nanoparticles. This proposed method of size-shrinking could be developed as a general strategy for large-scale tuning the properties of copper nanoparticles for wide applications and extended to other metal particles as well.