Methane (CH4) is the second greenhouse gas and has a profound impact on global climate change due to its high global warming potential and concentration. By 2022, the CH4 concentration was approximately 1.9 ppm, which was 264% of the pre-industrial level. The spatiotemporal distribution of CH4 was investigated by a portable CH4 detector on an unmanned aerial vehicle and electric bicycles in Shaoxing, a city situated in the Yangtze River Delta, China. The vertical distribution revealed CH4 concentration generally decreased slowly with height. However, the inversion condition and low atmospheric boundary layer height (ABLH) leaded to the enhancement of CH4 with height. The highest CH4 concentration (2.2 ± 0.1 ppm, n = 1428) was observed in winter and the lowest (2.0 ± 0.2 ppm, n = 1530) in spring. Regarding the daily variation, CH4 concentration peaked at 5:00 local time (LT) and reached its lowest level at 14:00 LT, which was attributed to the daily variation of ABLH, lowest in the early morning and highest in the noon. In urban areas, CH4 concentrations showed higher levels near restaurants, natural gas stations and sewerage well, with a maximum value of 13.1 ppm, which was caused by CH4 emission and natural gas leakage from these places. The annual CH4 emission in Shaoxing were estimated to be approximately 69 ton/(km2·year) by the mass balance approach. Compared with other cities in the world, the CH4 emission is in higher level which imply some control measures should be conducted to reduce CH4 emission in Shaoxing.