The cultivation of crop sunflower or Helianthus annuus is a 20 billion USD industry globally. Crop wild relatives of H. annuus have a long history of being used to breed improved traits into cultivated varieties. Cultivated H. annuus is not known to have a pleasant aroma, and at times seed yield is limited by pollination services, particularly in the production of hybrid seed. Improved floral fragrance could improve pollinator attraction and would add value to ornamental sunflowers in the context of the cut-flower industry. If volatile organic compounds that together generate favorable scents are present in wild Helianthus species, they could be bred into domesticated varieties. In order to assess the diversity of floral fragrance available in crop wild relatives, 30 diverse accessions of wild Helianthus as well as seven varieties of H. annuus spanning a domestication gradient were grown in a greenhouse experiment and variation in floral volatiles was analyzed by solid phase microextraction-gas chromatography-mass spectrometry. While alpha-pinene made up a significant portion of the volatiles emitted for most taxa, there was substantial diversity present across the genus. Most volatiles emitted were found to be monoterpenoids with a significant share of sesquiterpenoids. Several wild accessions such as H. debilis subsp. tardiflorus and H. praecox subsp. praecox as well as open-pollinated domesticated accessions of H. annuus show promise for breeding for improved floral fragrance due to high volatile abundance and likely favorable compound compositions.