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BACKGROUND The severe acute respiratory syndrome coronavirus 2 (SARS-CoV-2) outbreak may motivate smokers to attempt to stop in greater numbers. However, given the temporary closure of UK stop smoking services and vape shops, smokers attempting to quit may instead seek out mobile health support, such as smartphone apps. OBJECTIVE We examined, using an interrupted time series approach, whether the SARS-CoV-2 outbreak has been associated with a step change or increasing trend in UK downloads of an otherwise popular smoking cessation app, Smoke Free. METHODS Data were from daily and nondaily adult smokers in the United Kingdom who had downloaded the Smoke Free app between January 1, 2020, and March 31, 2020 (primary analysis), and January 1, 2019, and March 31, 2020 (secondary analysis). The outcome variable was the number of downloads aggregated at the 12-hourly (primary analysis) or daily level (secondary analysis). The explanatory variable was the start of the SARS-CoV-2 outbreak, operationalized as March 1, 2020 (primary analysis), and January 15, 2020 (secondary analysis). Generalized additive mixed models adjusted for relevant covariates were fitted. RESULTS Data were collected on 45,105 (primary analysis) and 119,881 (secondary analysis) users. In both analyses, there was no evidence for a step change or increasing trend in downloads attributable to the start of the SARS-CoV-2 outbreak. Calculation of Bayes factors (BFs) indicated that the data for the primary analysis favored the null hypothesis compared with large associations (for level, BF=0.25; for slope, BF=0.26) but were insensitive to the detection of small associations (for level, BF=0.78; for slope, BF=1.35). CONCLUSIONS In the United Kingdom, between January 1, 2020, and March 31, 2020, and between January 1, 2019, and March 31, 2020, there was no evidence that the SARS-CoV-2 outbreak has been associated with a large step change or increasing trend in downloads of a popular smoking cessation app. Findings on the association of the SARS-CoV-2 outbreak with a small step change or increasing trend were inconclusive.