Advanced oxidation processes (AOPs) operating under neutral to alkaline conditions are highly desirable for industrial applications. This study focuses on the use of Cu-doped titanate (Cu-TNT) hollow nanoreactors to effectively degrade organic pollutants in a Fenton-like manner across a broad pH from 3 to 10. The resulting Cu-TNT material possessed a BET surface area of 391.2 m2/g and pores with sizes between 2 to 20 nm. Experimental results from Fenton-like reactions reveal that Cu-TNT exhibited superior catalytic activity and long-term stability in degrading methyl orange compared to Na-titanate, Fe-titanate, copper ions, cuprous chloride, and solid sphere Cu-doped titanate. Notably, Cu-TNT performed optimally at a pH of 9, with singlet oxygen (1O2) and hydroxyl radicals (•OH) being recognized as the main active components. The improved catalytic efficiency was due to the extensive surface area, efficient mass diffusion in limited space, and quick Cu(Ⅰ)/Cu(Ⅱ) transformations. This study provided a feasible pathway to develop Cu-based nanoreactors as heterogeneous catalysts for highly efficient AOPs.