A recent policy in the U.S. authorized monthly benefits from the Supplemental Nutrition Assistance Program (SNAP) to be used online to increase grocery access and promote healthy eating. This study examined online grocery attitudes and purchasing behaviors among low-income SNAP-eligible households with young children with and without online grocery experience. An explanatory sequential mixed methods design was used, including a survey informed by the theory of planned behavior (TPB) and focus groups conducted between November–March 2021. In the quantitative phase, 310 Maryland residents completed an online survey assessing TPB constructs (attitudes, social norms, perceived control), and food purchase frequency online and in-store. Subsequently, 42 participated in the qualitative phase. Online food selection and fees were a common obstacle to online grocery purchasing. Families who had purchased groceries online (57%) had more positive attitudes and perceived fewer barriers to online shopping than those who had not. Self-reported frequency of buying fresh produce, meat and seafood, and sweets were lower online than in-store. Families discussed mistrust of online hired shoppers and fewer impulse purchases online as reasons for less frequent purchases of produce and sweets, respectively. Successful scale-up of the U.S. policy must address barriers to healthier purchasing behaviors to effectively promote equitable food access, such as decreasing delivery fees and improving the online food selection.

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