<b><i>Introduction:</i></b> This study aimed to estimate prevalence rates of mental health symptoms (anxiety, depression, and overall psychological distress) by tobacco smoking status, and associations between such symptoms and the level of dependence, motivation, and attempts to quit smoking in the German population. <b><i>Methods:</i></b> Cross-sectional analysis of data from six waves of a nationally representative household survey collected in 2018/19 (<i>N</i> = 11,937 respondents aged ≥18). Mental health symptoms were assessed with the Patient Health Questionnaire-4. Associations with smoking status, dependence, motivation to quit, and ≥1 past-year quit attempt (yes/no) were analysed with adjusted regression models among the total group, and among subgroups of current (<i>n</i> = 3,248) and past-year smokers (quit ≤12 months ago, <i>n</i> = 3,357). <b><i>Results:</i></b> Weighted prevalence rates of mental health symptoms among current, former, and never smokers were: 4.1%, 2.4%, 2.5% (anxiety), 5.4%, 4.7%, 4.0% (depression), and 3.1%, 2.5%, 2.4% (psychological distress). Current versus never smokers were more likely to report symptoms of anxiety and depression. Smokers with higher versus lower levels of dependence were more likely to report higher levels of all three mental health symptoms. Higher versus lower levels of overall psychological distress were associated with a higher motivation to quit smoking and, among past-year smokers, with higher odds of reporting a past-year quit attempt. <b><i>Conclusions:</i></b> We found various relevant associations between mental health symptoms and smoking behaviour. Healthcare professionals need to be informed about these associations and trained to effectively support this vulnerable group in translating their motivation into abstinence.