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Construction of highly efficient hollow nanosphere photocatalytic systems has been strongly attracting the attention of researchers. In the present work, nanopore enriched hollow carbon nitride nanospheres (HCNNSs) with a smaller particle size (200 nm) and a thinner shell thickness (40 nm) are successfully fabricated by a silica-nanocasting strategy. Such unique structures possess many advantages such as large BET surface area (122 m2 g−1), high light-harvesting ability, fast charge separation and transfer efficiency, plentiful exposed active sites and enhanced oxidation ability of photogenerated holes (h+VB). Therefore, HCNNSs in smaller sizes (HCNNS-200) exhibit extremely excellent visible-light photocatalytic efficiency towards the degradation of contaminants of emerging concern, e.g. levofloxacin (LEVO), in comparison with bulk g-C3N4 and HCNNSs in larger sizes (HCNNS-500). And it takes less than 10 min to finish the degradation of LEVO. The experimental results including those from indirect chemical probing, electron spin resonance, ion chromatography and high performance liquid chromatography-mass spectrometry confirm that h+VB and ˙O2− are the active species that are responsible for the mineralization of LEVO to NO3−, F−, H2O and CO2 under visible-light irradiation. Additionally, the degradation pathway of LEVO in the HCNNS-200 photocatalytic system is also proposed. It is expected that HCNNS-200 can be used as a promising photocatalyst for environmental remediation.