The study aimed to estimate dietary flavonol and flavone intakes and investigate major dietary sources by FFQ in Harbin of China. A total of 5,046 volunteers completed a semiquantitative food frequency questionnaire (FFQ). A random subsample of 167 healthy subjects completed the 7 consecutive 24-h dietary recalls and 2 FFQ for assessing the reproducibility and validity of FFQ. The correlation coefficients between 2 FFQ were 0.72 for flavonols and 0.65 for flavones; and between FFQ 2 and the 24-h dietary recall, they were 0.62 for flavonols and 0.58 for flavones. When flavonol and flavone intakes were categorized by quartile, complete and partial agreement ranged from 76% to 84%. The total intake of flavonols and flavones was 19.13 mg/day, and the mean flavonol and flavone intakes were 14.30 mg/day and 4.82 mg/day, respectively. Quercetin was the major contributor (31%) to total intake of flavonols and flavones, followed by kaempferol (22%). The main food sources of flavonols and flavones were apple (12%), potato (8%), celery (7%), eggplant (7%), and actinidia (5%). This work could facilitate the investigation on the proposed relation between these flavonoids and the prevention of chronic diseases.