Nighttime smartphone use is associated with sleep problems, which in turn have a bidirectional association with overweight. We aim to investigate whether nighttime smartphone use and sleep are related to overweight and metabolic dysfunction in adult populations. We used data from three population samples (aged 16–89) from the SmartSleep Study, which included survey data (N = 29,838), high-resolution tracking data (N = 3446), follow-up data (N = 1768), and cardiometabolic risk markers (N = 242). Frequent self-reported nighttime smartphone use was associated with 51% higher odds (95% CI: 1.32; 1.70) of overweight compared with no use. Tracked nighttime smartphone use was also associated with overweight. Similar results were found for obesity as an outcome. No consistent associations were found between nighttime smartphone use and cardiometabolic risk markers in a small subsample of healthy young women. Poor sleep quality (vs. good sleep quality) was associated with overweight (OR = 1.19, 85% CI: 1.10; 1.28). Overall, frequent nighttime smartphone use was consistently associated with overweight and a higher BMI across diverse population samples. The bidirectional interplay between nighttime smartphone use, sleep, and overweight may create a vicious circle of metabolic dysfunction over time. Therefore, nighttime smartphone use may be a potential target point for public health interventions to reduce overweight at the population level.