Being able to distinguish light-quark jets from gluon jets on an event-by-event basis could significantly enhance the reach for many new physics searches at the Large Hadron Collider. Through an exhaustive search of existing and novel jet substructure observables, we find that a multivariate approach can filter out over 95% of the gluon jets while keeping more than half of the light-quark jets. Moreover, a combination of two simple variables, the charge track multiplicity and the pT -weighted linear radial moment (girth), can achieve similar results. While this pair appears very promising, our study is only Monte Carlo based, and other discriminants may work better with real data in a realistic experimental environment. To that end, we explore many other observables constructed using different jet sizes and parameters, and highlight those that deserve further theoretical and experimental scrutiny. Additional information, including distributions of around 10,000 variables, can be found on the website http://jets.physics.harvard.edu/qvg.