This study assesses the associations of objectively-measured smartphone time with physical activity, sedentary behavior, mood, and sleep patterns among young adults by collecting real-time data of the smartphone screen-state. The sample consisted of 306 college-aged students (mean age ± SD: 20.7 ± 1.4 years; 60% males). Over seven days of time, the following variables were measured in the participants: objectively-measured smartphone use (Your Hour and Screen Time applications), objective and subjective physical activity (GoogleFit and Apple Health applications, and the International Physical Activity Questionnaire (IPAQ), respectively), the number of hours sitting (IPAQ), mood (The Profile of Mood State (POMS)), and sleep (The Pittsburgh Sleep Quality Index (PSQI)). Multiple regressions analyses showed that the number of hours sitting per day, physical activity, and the POMS Global Score significantly predicted smartphone use (adj.R2 = 0.15). Further, participants with low levels of physical activity were more likely to increase the use of smartphones (OR = 2.981). Moreover, mood state (β = 0.185; 95% CI = 0.05, 0.32) and sleep quality (β = 0.076; 95% CI = −0.06, 0.21) predicted smartphone use, with those reporting poor quality of sleep (PSQI index >5) being more likely to use the smartphone (OR = 2.679). In conclusion, there is an association between objectively-measured smartphone use and physical activity, sedentary behavior, mood, and sleep patterns. Those participants with low levels of physical activity, high levels of sedentary behavior, poor mood state, and poor sleep quality were more likely to spend more time using their smartphones.