The features detected in monolayer atmospheric columns sounded by the Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP) and classified as cloud or aerosol layers by the CALIOP version 4 (V4) cloud and aerosol discrimination (CAD) algorithm are reassessed using perfectly collocated brightness temperatures measured by the Imaging Infrared Radiometer (IIR) aboard the same satellite. Using the IIR's three wavelength measurements of layers that are confidently classified by the CALIOP CAD algorithm, we calculate two-dimensional (2-D) probability distribution functions (PDFs) of IIR brightness temperature differences (BTDs) for different cloud and aerosol types. We then compare these PDFs with 1-D radiative transfer simulations for ice and water clouds and dust and marine aerosols. Using these IIR 2-D BTD signature PDFs, we develop and deploy a new IIR-based CAD algorithm and compare the classifications obtained to the results reported by the CALIOP-only V4 CAD algorithm. IIR observations are shown to be able to identify clouds with a good accuracy. The IIR cloud identifications agree very well with layers classified as confident clouds by the V4 CAD algorithm (88 %). More importantly, simultaneous use of IIR information reduces the ambiguity in a notable fraction of "not confident" V4 cloud classifications. 28 % and 14 % of the ambiguous V4 cloud classifications are reclassified more appropriately as confident cloud layers through the use of the IIR observations in the tropics and in the midlatitudes, respectively. IIR observations are of relatively little help in deriving high-confidence classifications for most aerosols, as the low altitudes and small optical depths of aerosol layers yield IIR signatures that are similar to those of clear skies. However, misclassifications of aerosol layers, such as dense dust or elevated smoke layers, by the V4 CAD algorithm can be corrected to cloud layer classification by including IIR information. 10 %, 16 %, and 6 % of the ambiguous V4 dust, polluted dust, and tropospheric elevated smoke, respectively, are found to be misclassified cloud layers by the IIR measurements.