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• The concept of the SC in buildings coupling PCRs for atmosphere CH 4 removal was quantitively verified. • The effects of CH 4 degradation and indoor ventilation by the system were analyzed. • The photocatalytic efficiency, purification rate, and fresh air rate were analyzed. • The new system could degrade 57.27 μg/s of atmospheric CH 4 under optimal conditions. The techniques for the removal of methane from the atmosphere are highly challenging due to its stable chemical properties, dispersed sources, and low concentrations. This paper proposes a practical small-scale solar chimney (SC) in buildings with photocatalytic reactors (PCRs) for atmospheric methane removal. Two comprehensive numerical models on photocatalytic reaction and indoor ventilation are developed. The numerical simulation considers the performance of methane removal and indoor air ventilation of the proposed system, as well as its specific crucial parameters such as the type of PCRs, solar radiation, and flow channel width. The obtained results show that the SC with honeycomb photocatalytic reactor (HPCR) is more able to remove atmospheric methane than SC with plate photocatalytic reactor (PPCR) under the premise of meeting the ventilation standards. In addition, there is a maximum methane purification rate of 57.27 μg/s under the condition that the air gap width is 0.3 m, the length of the HPCR is 1.5 m, and the porosity is 0.85. It is then proved that the SC in buildings with PCRs can allow small-scale, zero-energy consumption, continuable, and decentralized low-concentration atmospheric methane removal while improving the indoor ventilation. [ABSTRACT FROM AUTHOR]