A Tethered balloon-based field campaign was launched for the vertical observation of air pollutants within the lower troposphere of 1000 m for the first time over a Chinese megacity, Shanghai in December of 2013. A custom-designed instrumentation platform for tethered balloon observation and ground-based observation synchronously operated for the measurement of same meteorological parameters and typical air pollutants. One episodic event (December 13) was selected with specific focus on particulate black carbon, a short-lived climate forcer with strong warming effect. Diurnal variation of the mixing layer height showed very shallow boundary of less than 300 m in early morning and night due to nocturnal inversion while extended boundary of more than 1000 m from noon to afternoon. Wind profiles showed relatively stagnant synoptic condition in the morning, frequent shifts between upward and downward motion at noon and in the afternoon, and dominant downward motion with sea breeze in the evening. Characteristics of black carbon vertical profiles during four different periods of a day were analyzed and compared. In the morning, surface BC concentration averaged as high as 20 μg/m3 due to intense traffic emissions from the morning rush hours and unfavorable meteorological conditions. A strong gradient of BC concentrations with altitude was observed from the ground to the top of boundary layer at around 250-370 m. BC gradients turned much smaller above the boundary layer. BC profiles measured during noon and afternoon were the least dependent on heights. The largely extended boundary layer with strong vertical convection was responsible for a well mixing of BC particles in the whole measured column. BC profiles were similar between the early-evening and late-evening phases. The lower troposphere was divided into two stratified air layers with contrasted BC vertical distributions. Profiles at night showed strong gradients from the relatively high surface concentrations to low concentrations near the top of the boundary layer around 200 m. Above the boundary layer, BC increased with altitudes and reached a maximum at the top of 1000 m. Prevailing sea breeze within the boundary layer was mainly responsible for the quick cleanup of BC in the lower altitudes. In contrast, continental outflow via regional transport was the major cause of the enhanced BC aloft. This study provides a first insight of the black carbon vertical profiles over Eastern China, which will have significant implications for narrowing the gaps between the source emissions and observations as well as improving estimations of BC radiative forcing and regional climate.