This dataset consists of 4,397 insect species associated with 679 native plant species, 120 archaeophytes, and 234 neophytes from the Database of Insects and their Food Plants (DBIF). The DBIF details approximately 60,000 interactions between phytophagous insect (and mite) species and plants recorded in Great Britain over the last century, based on a wide variety of sources, including entomological journals and field guides. The data here represents a reduced subset of the full DBIF (13,277 interactions), only including interactions resolved to the species level (insect species x associated with host plant species y), records that have been expertly verified as reliable and included in previous large-scale analyses (Ward 1988; Ward & Spalding 1993; Ward et al. 1995; Ward et al. 2003), and records that are certain to have occurred in Great Britain. Any records originating from captive breeding studies are excluded. Finally, only plants with associated phylogenetic data and native status are included. Host plant distribution size is also included, in addition to a quantification of the distinctiveness of the insect communities found on a subset of the non-native plants. This work was supported by the Natural Environment Research Council award number NE/R016429/1 as part of the UK-SCAPE programme delivering National Capability. Full details about this dataset can be found at https://doi.org/10.5285/33a825f3-27cb-4b39-b59c-0f8182e8e2e4