This dataset holds in situ sound recordings from sites in Greater Cape Floristic Region (GCFR), South Africa from June to December 2023. The recordings were collected as part of the Biodiversity Survey of the Cape (BioSCape) project, a multi-agency, NASA-led research project that integrates airborne imaging spectroscopy and lidar with a suite of measurements of biodiversity. BioSoundSCape is a BioSCape subproject seeking to relate ground-based measures of bioacoustic diversity to remote imagery. AudioMoth recorders were deployed at sites for 4 to 10 days of data collection (median = 7), and programmed to record 1 min of every 10, thus providing temporal sampling through day and night. Each recording was saved in a waveform audio file format with 16-bit digitization depth and a 48 kHz sampling rate. The recordings contain a wide range of environmental sounds such as biophony (e.g., birds, frogs, insects), anthropophony (e.g,. automobiles, airplanes) and geophony (e.g,. wind, rain). Sampling locations were stratified with respect to elevation, broad land use/land cover types, and time since wildfire disturbance. Most sites were within protected fynbos and Afromontane forest ecosystems. There were 505 sites in the wet season and 489 sites in the dry season, with most sites co-located between seasons. All sites were located within AVIRIS-NG hyperspectral acquisitions and 61% of sites were in LVIS lidar acquisitions. The dataset includes site information in tabular form and photographs of field sites.