The accurate and detailed measurement of the vertical temperature, humidity, pressure, and wind profiles of the atmosphere is pivotal for high-resolution numerical weather prediction, the determination of atmospheric stability, as well as investigation of small-scale phenomena such as urban heat islands. Traditional approaches, such as weather balloons, have been indispensable but are constrained by cost, environmental impact, and data sparsity. In this article, we investigate uncrewed aerial systems (UASs) as an innovative platform for in situ atmospheric probing. By comparing data from a drone-mounted semiconductor temperature sensor (TMP117) with traditional radiosonde measurements, we spotlight the UAS-collected atmospheric data’s accuracy and such system suitability for atmospheric surface layer measurement. Our research encountered challenges linked with the inherent delays in achieving ambient temperature readings. However, by applying specific data processing techniques, including smoothing methodologies like the Savitzky–Golay filter, iterative smoothing, time shift, and Newton’s law of cooling, we have improved the data accuracy and consistency. In this article, 28 flights were examined and certain patterns between different methodologies and sensors were observed. Temperature differentials were assessed over a range of 100 m. The article highlights a notable accuracy achievement of 0.16 ± 0.014 °C with 95% confidence when applying Newton’s law of cooling in comparison to a radiosonde RS41’s data. Our findings demonstrate the potential of UASs in capturing accurate high-resolution vertical temperature profiles. This work posits that UASs, with further refinements, could revolutionize atmospheric data collection.