Charge accumulates on an object due to friction, and can be quantified given the contact action as well as the material types. As long as a charged object doesn't touch ground in a vacuum, it would theoretically be able to acquire an infinite amount of charge. In reality, there is a breakdown of air that occurs when something has too much charge, which results in an electric arc.
The movement of charge, current, is what kills you - high power results in heat dissipation which can burn you. In addition, amperes passing through your body can disrupt your heartbeat and other electrical pathways in your body.
Van de Graaf generator revisited:
I was confused why we can touch a Van de Graaf generator and not get killed when we next contact ground. It turns out that air is more conducive than I gave it credit for. After touching the generator, you will discharge fast enough to not sustain injuries before you reach the ground.
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