This study develops the use of spectral total and diffuse irradiance measurements, made from a prototype hyperspectral total-diffuse sunshine pyranometer (SPN-S), to retrieve layer fine-mode aerosol (τaer) and total optical depths from airborne platforms. Additionally, we use spectral analysis in an attempt to partition the total optical depth into its τaer and cirrus cloud optical depth (τcld) components in the absence of coarse-mode aerosols. Two retrieval methods are developed: one leveraging information in the diffuse irradiance and the other using spectral characteristics of the transmitted direct beam, with each approach best suited for specific cloud and aerosol conditions. The SPN-S has advantages over traditional sun photometer systems, including no moving parts and a low cost. However, a significant drawback of the instrument is that it is unable to measure the direct-beam irradiance as accurately as sun photometers. To compensate for the greater measurement uncertainty in the radiometric irradiances, these retrieval techniques employ ratioed inputs or spectral information to reduce output uncertainty. This analysis uses irradiance measurements from the SPN-S and the solar spectral flux radiometer (SSFR) aboard the National Aeronautics and Space Administration's (NASA) P-3 aircraft during the 2018 deployment of the ObseRvations of Aerosols above CLouds and their intEractionS (ORACLES) campaign and the 2019 Cloud, Aerosol and Monsoon Processes Philippines Experiment (CAMP2Ex) mission to quantify above-aircraft cirrus τcld and derive vertical profiles of layer τaer. Validation of the τaer retrieval is accomplished by comparison with co-located measurements of direct solar irradiance made by the Sky-Scanning Sun-Tracking Atmospheric Research (4STAR) and in situ measurements of aerosol optical depth. For the aggregated 2018 ORACLES results, regression between the SPN-S-based method and sun photometer τaer values yields a slope of 0.96 with an R2 of 0.96, while the root mean square error (RMSE) is 3.0×10-2. When comparing the retrieved τaer to profiles of integrated in situ measurements of optical extinction, the slope, R2, and RMSE values for ORACLES are 0.90, 0.96, and 3.4×10-2, and for CAMP2Ex they are 0.94, 0.97, and 3.4×10-2, respectively. This paper is a demonstration of methods for deriving cloud and aerosol optical properties in environments where both atmospheric constituents may be present. With improvements to the low-cost SPN-S radiometer instrument, it may be possible to extend these methods to a broader set of sampling applications, such as ground-based settings.