A high-resolution positron emission tomography (PET)- and magnetic resonance imaging-based human brain atlas of four important serotonin receptors (5-HT1A, 5-HT1B, 5-HT2A, 5-HT4) and the serotonin transporter (5-HTT) is presented. The actual dataset includes five NIfTI images (one NIfTI for each serotonin tracer) and 10 FreeSurfer surfaces with average non-displaceable binding potential (BPND) values (two Freesurfer surfaces for each serotonin tracer). The molecular imaging maps were related to autoradiography data and an unprecedented agreement was found, supporting the validity of the methodology and results presented, and allowing translating PET binding estimates into densities. This conversion facilitates the interpretability of the maps and allows for a direct comparison across the five 5-HT targets, in vivo in the human brain. All participants included in this study were healthy male and female controls from the Cimbi database; the data analysis was restricted to include individuals aged between 18 and 45 years. A total of 232 PET scans and corresponding structural MRI scans were acquired for 210 individual participants; 189 subjects had only one scan, 20 subjects had two scans, and a single had three scans. Scans were combined and aggregated atlases for each serotonin tracer were generated. For more information on the original data, please go to: https://xtra.nru.dk/FS5ht-atlas/