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Background Online grocery delivery services (OGDSs) are a popular way of acquiring food. However, it is unclear whether OGDS use is associated with the healthiness of purchases and whether there are sociodemographic differences in OGDS use. If so, the increased prevalence of OGDS use may have implications for population diet, and differential OGDS use could contribute to diet inequalities. Objective This study aimed to examine whether OGDS use varies by sociodemographic characteristics and is associated with the amount and types of groceries purchased. Methods Item-level take-home food and drink purchase data (n= 3,233,920 items) from households in London and the North of England were available from the 2019 UK Kantar fast-moving consumer goods panel (N= 1911). Purchases were categorized as being bought online or in-store. We used logistic regression to estimate the likelihood of an above-median frequency of OGDS use by sociodemographic characteristics. We used Poisson regression to estimate the differences in energy and nutrients purchased by households that had above-and below-median OGDS use and the proportion of energy purchased from products high in fat, salt, and sugar (HFSS) online versus in-store among households that used both shopping methods (n= 665). Results In total, 668 (35%) households used OGDSs at least once in 2019. Of the households that used OGDSs, the median use was 5 occasions in 2019. Households were more likely to have above-median use in London versus in the North of England (odds ratio 1.29, 95% CI 1.01-1.65) and if they had a higher annual household …