Fundamental insight on predator-prey dynamics in the deep sea is hampered by a lack of combined data on hunting behavior and prey spectra. Deep-sea niche segregation may evolve when predators target specific prey communities, but this hypothesis remains untested. We combined environmental DNA (eDNA) metabarcoding with biologging to assess cephalopod community composition in the deep-sea foraging habitat of two top predator cetaceans. Here, we are presenting the eDNA data from seawater samples obtained during a cruise on RV Pelagia in 2018 off Terceira, Azores, sampled directly in the foraging habitats of two cetacean top-predators from the surface to 1600 m. The water was collected using Niskin bottles mounted on a CTD rosette at seven or eight depths in biological triplicates and filtered on sterile Sterivex filter. After DNA extraction and PCR amplification with two universal cephalopod primer (Ceph18S, targeting the nuclear 18S rRNA gene and CephMLS targeting the mitochondrial 16S rRNA gene), the samples were sequenced on an Illumina MiSeq with the MiSeq Reagent kit v3 (600 cycles).