This data set contains raw, annotated, and synthesized data used in the analysis by Hinke et al. (2021) titled "Serendipitous observations from animal-borne video loggers reveal synchronous diving and equivalent prey capture rates in chinstrap penguins" (DOI:10.1007/s00227-021-03937-5). The data derive from field work to monitor the diving and predation behaviors of two chinstrap penguins (Pygoscelis antarcticus) from Cape Shireff, Livingston Island (60.79°W, 62.46°S) in Antarctica. Sampling occurred from 20 December 2019 to 31 Jan 2020. The raw data include the video files and complete dive records from the deployment of animal-borne video loggers and time-depth recorders on two individual chinstrap penguins. The videos are recorded in 30-minute clips and encompass over 4.5 hours of observation for each bird. Five independent, manual annotations of each video, transcribed onto the corresponding time-depth records of each bird, respectively, document the diving and predation events observed in each video. A separate annotation file that records the presence of companion birds in each video is also included. Additionally, we include two files that were generated during the analysis of the data. The first merges each (N=5) annotation of krill consumption and dive duration for each synchronous dive. The second merges select dive characteristics from each synchronous dive. Finally, we include data on the lengths of krill eaten by penguins during the study period. The krill length data were collected via gastric lavage to characterize the prey field that was encountered by foraging penguins during the sampling season. A READ ME file fully documents each file and important header information.