Background: Previous studies have identified psychological and smartphone app–related predictors of engagement with alcohol reduction apps at a group level. However, strategies to promote engagement need to be effective at the individual level. Evidence as to whether group-level predictors of engagement are also predictive for individuals is lacking. Objective: The aim of this study was to examine whether daily fluctuations in (1) the receipt of a reminder, (2) motivation to reduce alcohol, (3) perceived usefulness of the app, (4) alcohol consumption, and (5) perceived lack of time predicted within-person variability in the frequency and amount of engagement with an alcohol reduction app. Methods: We conducted a series of observational N-of-1 studies. The predictor variables were measured twice daily for 28 days via ecological momentary assessments. The outcome variables were measured through automated recordings of the participants’ app screen views. A total of nine London-based adults who drank alcohol excessively and were willing to set a reduction goal took part. Each participant’s dataset was analyzed separately using generalized additive mixed models to derive incidence rate ratios (IRRs) for the within-person associations of the predictor and outcome variables. Debriefing interviews, analyzed using thematic analysis, were used to contextualize the findings. Results: Predictors of the frequency and amount of engagement differed between individuals, and for the variables ‘perceived usefulness of the app’ and ‘perceived lack of time’, the direction of associations also differed between individuals. The most consistent predictors of within-person variability in the frequency of engagement were the receipt of a daily reminder (IRR=1.80-3.88; P<.05) and perceived usefulness of the app (IRR=0.82-1.42; P<.05). The most consistent predictors of within-person variability in the amount of engagement were motivation to reduce alcohol (IRR=1.67-3.45; P<.05) and perceived usefulness of the app (IRR=0.52-137.32; P<.05). Conclusions: The utility of the selected psychological and app-related variables in predicting the frequency and amount of engagement with an alcohol reduction app differed at the individual level. This highlights that key within-person associations may be masked in group-level designs and suggests that different strategies to promote engagement may be required for different individuals.