The vertical distribution profiles of NO <sub xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">2</sub> are essential for understanding the mechanisms, detecting near-surface emissions, and tracking pollutant transportation at high altitude. However, most of the published NO <sub xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">2</sub> studies are based on the surface 2-D measurements. The ground-based 3-D remote-sensing stations were recently built to measure vertical distribution profiles of NO <sub xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">2</sub> . However, the stations were spatially sparse due to the high cost and could not make the measurements without sunlight. In this study, we first developed a multimodel fusion network (MF-net) based on the sparse vertical observations from the Jing-Jin-Ji region. We achieved the 3-D profile prediction of NO <sub xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">2</sub> in the range of 39.005–41.405N and 115.005–117.905E with 24-h coverage. The MF-net significantly surpassed the conventional WRF-CHEM model and provided a more accurate evaluation of the NO <sub xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">2</sub> transmission between Beijing and the neighboring cities. Besides, the MF-net covers the monitoring of NO <sub xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">2</sub> to the whole study area and extends the monitoring time to the entire day (24 h), making it serviceable for continuous spatial-temporal estimation of NO <sub xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">2</sub> and its transmission in pollution events. The MF-net provides more robust data support to formulate reasonable and effective pollution prevention and control measures.