In this research dataset, we summarize for the first time volatile organic compounds (VOCs) emitted in vivo from ripening wine grapes. We studied four cold-hardy cultivars grown in the Midwestern U.S.: St. Croix, Frontenac, Marquette, and La Crescent. These cultivars have gained popularity among local growers and winemakers, but still very little is known about their performance compared with long-established V. viniferagrapes. Volatiles were collected using two novel approaches: biogenic emissions from grape clusters on a vine and single grape berries. A third approach was headspace collection of volatiles from crushed grapes. Solid-phase microextraction (SPME) was used to collect volatiles. Vacuum-assisted SPME was used in the case of single grape berry. Collected VOCs were analyzed using separation and identification on a gas chromatograph mass spectrometer (GC-MS). More than 120 VOCs were identified using mass spectral libraries. The dataset provides evidence that detecting biogenic emissions from growing grapes is feasible. The dataset provides a record of temporal and spatial variability of VOCs, many of which could potentially impart aroma and flavor in the wine. The number of VOCs detected followed the order from single berry (the least) to crushed berry (the most). Thus, more information for potential use in harvesting in order to obtain the desired flavor is found in data from crushed grapes.