The around-the-clock smartphone use and its relation to disturbed sleep is a public health concern. The present study aimed to quantify the effects of different dimensions of smartphone behaviours (frequency of daytime use, problematic use, use before sleep and use during the sleep period) on disturbed sleep (sleep quality and sleep quantity) and to disentangle their inter-relationship in a large population-based sample of 24,856 Danish adults aged >= 16 years. Data come from the SmartSleep Experiment, which is a web-based survey carried out using a citizen science approach. Tested items were used to evaluate smartphone use and disturbed sleep was evaluated with the Karolinska Sleep Questionnaire (KSQ). Linear and multinomial logistic regression was employed to evaluate the relationship between smartphone use and disturbed sleep. While several of the smartphone measures were associated with disturbed sleep when assessed individually, smartphone use during the sleep period was the only dimension consistently associated with disturbed sleep when assessed independently of other smartphone behaviours. Weekly smartphone use during the sleep period versus no use was associated on average with a 0.96 point higher score (95% confidence interval [CI] 0.90-1.02) on the 5-point KSQ scale, and a higher risk of both short (odds ratio [OR] 1.32, 95% CI 1.08-1.62) and long (OR 1.94, 95% CI 1.63-2.32) sleep duration. Smartphone use during the sleep period is the factor strongest associated to disturbed sleep relative to other dimensions of smartphone use. Recommendations around smartphone use during the sleep period are warranted in order to protect the fundamentally important biological and mental processes of sleep.