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In the present study, N-doped hollow carbon nanospheres (NHCNs) were synthesized with a combined soft template-chemical activation method. Spherical hollow hydrochar was prepared from glucose with the assistance of dual soft templates, and was then chemically activated with KHCO 3 and urea to produce the NHCNs. Effects of urea addition and activation temperature on the NHCNs' physicochemical properties were revealed. The NHCNs were endowed with rich N-doping and developed porosity. The sample activated at 800 °C (NHCN2800) showed an impressive specific surface area of 3234 m2/g. The proposed method could also be extended to the synthesis of N, S co-doped hollow carbon nanospheres. We then investigated CO 2 adsorption performances of the NHCNs. At 25 °C and 1 bar, the best CO 2 uptake of the NHCNs was 4.36 mmol/g; at 20 bar, it increased to a record high level of 23.62 mmol/g. Correlations between textural characteristics/N-doping and CO 2 adsorption at 1/20 bar were analyzed and discussed. The current study indicated that the obtained NHCNs had great potential for applications in both pre- and post-combustion CO 2 capture. [Display omitted] • NHCNs are prepared with a combined soft template-chemical activation method. • The NHCNs demonstrate well-defined hollow spherical structure. • The NHCNs exhibit ultrahigh S BET up to 3234 m2/g. • At 25 °C and 20 bar, CO2 uptake of the NHCNs reaches 23.62 mmol/g. [ABSTRACT FROM AUTHOR]