The aims of this study were to evaluate spectral detector CT (SDCT)-derived iodine concentration (IC) of lymph nodes diagnosed as metastatic and benign in prostate-specific membrane antigen (PSMA) PET/CT and to assess its potential use for lymph node assessment in prostate cancer. Thirty-four prostate cancer patients were retrospectively included: 16 patients with and 18 without lymph node metastases as determined by PSMA PET/CT. Patients underwent PSMA PET/CT as well as portal venous phase abdominal SDCT for clinical cancer follow-up. Only scan pairs with a stable nodal status indicated by constant size as well as comparable prostate-specific antigen (PSA) levels were included. One hundred benign and 96 suspected metastatic lymph nodes were annotated and correlated between SDCT and PSMA PET/CT. Iodine concentration in SDCT-derived iodine maps and SUVmax in ultra-high definition reconstructions from PSMA PET/CT were acquired based on the region of interest. Metastatic lymph nodes as per PSMA PET/CT showed higher IC than nonmetastatic nodes (1.9 ± 0.6 mg/mL vs 1.5 ± 0.5 mg/mL, P < 0.05) resulting in an AUC of 0.72 and sensitivity/specificity of 81.3%/58.5%. The mean short axis diameter of metastatic lymph nodes was larger than that of nonmetastatic nodes (6.9 ± 3.6 mm vs 5.3 ± 1.3 mm; P < 0.05); a size threshold of 1 cm short axis diameter resulted in a sensitivity/specificity of 12.8%/99.0%. There was a significant yet weak positive correlation between SUVmax and IC (rs = 0.25; P < 0.001). Spectral detector CT-derived IC was increased in lymph nodes diagnosed as metastatic in PSMA PET/CT yet showed considerable data overlap. The correlation between IC and SUVmax was weak, highlighting the role of PSMA PET/CT as important reference imaging modality for detection of lymph node metastases in prostate cancer patients.