Background: Substance use disorders are reliably associated with high impulsivity and sensation seeking. Importantly, both precede problematic substance use, implicating them as risk factors. Individuals with substance use disorders show variable degrees of substance use (combined quantity and frequency) and substance-related problems and differ in both aspects from healthy controls. Dimensional research has indicated differential associations of impulsivity-related traits as well as sensation seeking with the degree of substance use and substance-related problems. The current study aimed to clarify whether impulsivity-related traits and sensation seeking predict substance-related problems above and beyond the degree of substance use and are thus specifically linked to problems, the dimension that characterizes substance use disorders. Method: We assessed impulsivity-related traits and sensation seeking using self-report, as well as delay discounting, a behavioral indicator of impulsivity, in a sample of 258 substance-using adults. Results: Sensation seeking and impulsivity-related traits significantly predicted the degree of substance use, with sensation seeking explaining the largest portion of variance. In contrast, self-reported impulsivity, in particular when experiencing negative emotions (urgency), but not sensation seeking or delay discounting, predicted substance-related problems when controlling for the degree of substance use. Conclusions: This suggests that urgency, but not sensation seeking, may be specifically linked to substance-related problems and thus especially relevant for substance use disorders. Taken together, this study underlines the necessity to assess and control for the degree of substance use in risk factor research concerning substance-related problems. Thus, it may inform future research improving targeted prevention and therapy.