A recent report noted that 93.4% of Peruvian citizens own a smartphone and that this has impacted positively in society for different purposes. Despite its advantages, scholars and practitioners have been investigating human-Technology interaction, psychological processes, and their possible negative effects. Previous studies have investigated Problematic Mobile Phone Use (PMPU) as a dysfunctional interaction concerning the excessive use of smartphone activities that results progressively in negative consequences such as lack of control, preoccupation, withdrawal, relapse, and conflict. Despite this emergent area of research, there is little research examining PMPU among young Peruvian adults. In addition to this, there are still inconsistencies in relationship between PMPU, and substance use, and other risky behaviors. This paper analyses the impact of smartphone usage patterns, sensation seeking, and substance use in relation to PMPU. A total of 921 college students from Peru were recruited and completed a survey examining demographics, usage patterns, sensation seeking, and substance use. Overall, results indicate that gender, time spent talking on mobile phones, sensation seeking, and psychoactive substance use were predictors of PMPU. Implications at a theoretical, practical, and methodological level are discussed in relation to further research of PMPU in Peru.